When the operating temperature of a solid oxide electrolysis cell(SOEC)is lower than the outlet temperature of a nuclear reactor,the reactor can be directly coupled with the SOEC as a high-temperature heat source.Howe...When the operating temperature of a solid oxide electrolysis cell(SOEC)is lower than the outlet temperature of a nuclear reactor,the reactor can be directly coupled with the SOEC as a high-temperature heat source.However,the key to the efficiency and return on investment of this hybrid energy system lies in the expected lifetime of the SOEC.This study assessed Ni-YSZ|YSZ|GDC|LSC fuel electrode support cells’long-term stability during electrolysis at 650℃with a current density of−0.5Acm^(−2)over 1818 h.The average voltage degradation rate of 2.63%kh^(−1)unfolded in two phases:an initial rapid decay(90 to 1120 h at 3.58%kh^(−1))and a stable decay(1120 to 1818 h at 2.14%kh^(−1)),emphasizing SOECs’probability coupling with nuclear reactors at 650℃.Post-1818-hour electrolysis revealed nickel particle formation associated with Ni(OH)_(x)diffusion and re-deposition,alongside a strontium-containing layer causing interface cracking.Despite minimal strontium segregation in the EDS,XPS data indicated surface segregation of Sr.This study provides crucial insights into prolonged SOEC operation,highlighting both its potential and challenges.展开更多
Driven by the global energy transition and carbon neutrality targets,alkaline water electrolysis has emerged as a key technology for coupling variable renewable generation with clean hydrogen production,offering consi...Driven by the global energy transition and carbon neutrality targets,alkaline water electrolysis has emerged as a key technology for coupling variable renewable generation with clean hydrogen production,offering considerable potential for absorbing surplus power and enhancing grid flexibility.However,conventional control architectures typically treat the power converter and electrolyzer as independent units,neglecting their dynamic interactions and thereby limiting overall system performance under practical operating conditions.This review critically examines existing control approaches,ranging from classical proportional-integral schemes to model predictive control,fuzzy-logic algorithms,and data-driven methods,evaluating their effectiveness in managing dynamic response,multivariable coupling,and operational constraints as well as their inherent limitations.Attention is then focused on the performance requirements of the hydrogen-production converter,including current ripple suppression,rapid transient response,adaptive thermal regulation,and stable power delivery.An integrated co‑control framework is proposed,aligning converter output with electrolyzer demand across steady-state operation,variable renewable input,and emergency shutdown scenarios to achieve higher efficiency,extended equipment lifetime,and enhanced operational safety.Finally,prospects for advancing unified control methodologies are outlined,with emphasis on constraint-aware predictive control,machine-learning-enhanced modeling,and real‑time co‑optimization for future alkaline electrolyzer systems.展开更多
Electrocatalytic water splitting for green hydrogen is hindered by the slow oxygen evolution reaction(OER).Replacing OER with ethylene glycol oxidation(EGOR)offers an energy-saving route,coproducing valuable chemicals...Electrocatalytic water splitting for green hydrogen is hindered by the slow oxygen evolution reaction(OER).Replacing OER with ethylene glycol oxidation(EGOR)offers an energy-saving route,coproducing valuable chemicals,but requires efficient,stable,and low-cost catalysts.Here,we report a sulfate-doped NiOOH-Ni(OH)_(2)catalyst(denoted S-NiOOH-Ni(OH)_(2)).SO_(4)^(2-)doping significantly boosts intrinsic activity,enabling exceptional EGOR performance(only 1.45 V for~650 mA cm^(-2)).In situ studies reveal that a unique"structural locking"effect stabilizes the highly activeβ-NiOOH phase within the composite,differing from conventional reconstruction.Notably,we successfully scaled up this catalyst to an industrial-scale electrolyzer(anode area:1386 cm^(2))and constructed an integrated electrochemical-conventional chemical coupling system,which stably produced 290 L of hydrogen and kilogram-scale high-purity potassium diformate(KDF)per batch.Techno-economic analysis confirms strong commercial viability,projecting$7.1 million annual profit and a payback period under one year.This work bridges advanced catalyst design to industrial biomass valorization coupled with hydrogen production.展开更多
The efficient storage and release of H_(2)are pivotal for the advancement of hydrogen energy technologies.Cyclohexane,as a promising liquid organic hydrogen carrier(LOHC),provides a safe and practical solution for H_(...The efficient storage and release of H_(2)are pivotal for the advancement of hydrogen energy technologies.Cyclohexane,as a promising liquid organic hydrogen carrier(LOHC),provides a safe and practical solution for H_(2)storage.However,the performance limitations of dehydrogenation catalysts have hindered the rapid development of LOHC technology.In this study,we successfully developed boron-modified Pt/ZrO_(2)catalysts,which exhibit exceptional catalytic performance in cyclohexane dehydrogenation.The optimal boron content is determined to be 0.5 wt.%,with the Pt/0.5B–ZrO_(2)catalyst achieving high turnover frequency(TOF)of 10,627.3 mol_(H_(2))·mol_(Pt)^(−1)·h^(−1)and benzene selectivity of 99%at 295°C.The catalyst also demonstrates H_(2)evolution rate of 908 mmol·g_(Pt)^(−1)·min^(−1)and low deactivation rate of 0.0043 h^(−1).Remarkably,the catalyst displays outstanding stability and regeneration performance,maintaining its activity without significant loss during a 60-h dehydrogenation reaction and retaining a cyclohexane conversion of 77.2%after 10 consecutive cycles.Comprehensive characterization techniques,including XPS,CO-FTIR,NH_(3)-TPD,H_(2)-TPD,Benzene-TPD,and Py-IR,reveals that boron modification reduces the electron density of Pt,generating abundant electron-deficient Pt atoms.These electron-deficient Pt atoms enhance H_(2)adsorption and accelerate benzene desorption,effectively preventing coke formation from deep benzene dehydrogenation,which is responsible for the high catalytic performance of the Pt/0.5B–ZrO_(2)catalyst.These findings offer a valuable strategy for optimizing dehydrogenation catalysts in LOHC technologies,addressing a critical bottleneck in the development of this essential energy storage solution.展开更多
The transition of hydrogen sourcing from carbon-intensive to water-based methodologies is underway,with renewable energy-powered proton exchange membrane water electrolysis(PEMWE)emerging as the preeminent pathway for...The transition of hydrogen sourcing from carbon-intensive to water-based methodologies is underway,with renewable energy-powered proton exchange membrane water electrolysis(PEMWE)emerging as the preeminent pathway for hydrogen production.Despite remarkable advancements in this field,confronting the sluggish electrochemical kinetics and inherent high-energy consumption arising from deteriorated mass transport within PEMWE systems remains a formidable obstacle.This impediment stems primarily from the hindered protons mass transfer and the untimely hydrogen bubbles detachment.To address these challenges,we harness the inherent variability of electrical energy and introduce an innovative pulsed dynamic water electrolysis system.Compared to constant voltage electrolysis(hydrogen production rate:51.6 m L h^(-1),energy consumption:5.37 kWh Nm-^(3)H_(2)),this strategy(hydrogen production rate:66 m L h^(-1),energy consumption:3.83 kWh Nm-^(3)H_(2))increases the hydrogen production rate by approximately 27%and reduces the energy consumption by about 28%.Furthermore,we demonstrate the practicality of this system by integrating it with an off-grid photovoltaic(PV)system designed for outdoor operation,successfully driving a hydrogen production current of up to 500 mA under an average voltage of approximately 2 V.The combined results of in-situ characterization and finite element analysis reveal the performance enhancement mechanism:pulsed dynamic electrolysis(PDE)dramatically accelerates the enrichment of protons at the electrode/solution interface and facilitates the release of bubbles on the electrode surface.As such,PDE-enhanced PEMWE represents a synergistic advancement,concurrently enhancing both the hydrogen generation reaction and associated transport processes.This promising technology not only redefines the landscape of electrolysis-based hydrogen production but also holds immense potential for broadening its application across a diverse spectrum of electrocatalytic endeavors.展开更多
Hydrogen energy from electrocatalysis driven by sustainable energy has emerged as a solution against the background of carbon neutrality.Proton exchange membrane(PEM)-based electrocatalytic systems represent a promisi...Hydrogen energy from electrocatalysis driven by sustainable energy has emerged as a solution against the background of carbon neutrality.Proton exchange membrane(PEM)-based electrocatalytic systems represent a promising technology for hydrogen production,which is equipped to combine efficiently with intermittent electricity from renewable energy sources.In this review,PEM-based electrocatalytic systems for H2 production are summarized systematically from low to high operating temperature systems.When the operating temperature is below 130℃,the representative device is a PEM water electrolyzer;its core components and respective functions,research status,and design strategies of key materials especially in electrocatalysts are presented and discussed.However,strong acidity,highly oxidative operating conditions,and the sluggish kinetics of the anode reaction of PEM water electrolyzers have limited their further development and shifted our attention to higher operating temperature PEM systems.Increasing the temperature of PEM-based electrocatalytic systems can cause an increase in current density,accelerate reaction kinetics and gas transport and reduce the ohmic value,activation losses,ΔGH*,and power consumption.Moreover,further increasing the operating temperature(120-300℃)of PEM-based devices endows various hydrogen carriers(e.g.,methanol,ethanol,and ammonia)with electrolysis,offering a new opportunity to produce hydrogen using PEM-based electrocatalytic systems.Finally,several future directions and prospects for developing PEM-based electrocatalytic systems for H_(2) production are proposed through devoting more efforts to the key components of devices and reduction of costs.展开更多
Electrocatalytic urea wastewater treatment technology has emerged as a promising method for environmental remediation.However,the realization of highly efficient and scalable electrocatalytic urea wastewater treatment...Electrocatalytic urea wastewater treatment technology has emerged as a promising method for environmental remediation.However,the realization of highly efficient and scalable electrocatalytic urea wastewater treatment(SEUWT)is still an enormous challenge.Herein,through regulating the adsorption behavior of urea functional groups,the efficient SEUWT coupled hydrogen production is realized in anion exchange membrane water electrolyzer(AEMWE).Density functional theory calculations indicate that self-driven electron transfer at the heterogeneous interface(NiO/Co_(3)O_(4))can induce charge redistribution,resulting in electron-rich NiO and electron-deficient Co_(3)O_(4),which are superior to adsorbing C=O(electron-withdrawing group)and–NH_(2)(electron-donating group),respectively,regulating the adsorption behavior of urea molecule and accelerating the reaction kinetics of urea oxidation.This viewpoint is further verified by temperature-programmed desorption experiments.The SEUWT coupled hydrogen production in AEMWE assembled with NiO/Co_(3)O_(4)(anode)and NiCoP(cathode)can continuously treat urea wastewater at an initial current density of 600 mA cm^(-2),with the average urea treatment efficiency about 53%.Compared with overall water splitting,the H_(2) production rate(8.33 mmol s^(-1))increases by approximately 3.5 times.This work provides a cost-effective strategy for scalable purifying urea-rich wastewater and energy-saving hydrogen production.展开更多
Establishing an energy-saving and affordable hydrogen production route from infinite seawater presents a promising strategy for achieving carbon neutrality and low-carbon development.Compared with the kinetically slug...Establishing an energy-saving and affordable hydrogen production route from infinite seawater presents a promising strategy for achieving carbon neutrality and low-carbon development.Compared with the kinetically sluggish oxygen evolution reaction(OER),the thermodynamically advantageous sulfion oxidation reaction(SOR)enables the S^(2-)pollutants recovery while reducing the energy input of water electrolysis.Here,a nanoporous NiMo alloy ligament(np-NiMo)with AlNi_(3)/Al_(5)Mo heterostructure was prepared for hydrogen evolution reaction(HER,-0.134V versus reversible hydrogen electrode(vs.RHE)at 50mA/cm^(2)),which needs an Al_(89)Ni_(10)Mo_(1)as a precursor and dealloying operation.Further,the np-NiMo alloy was thermal-treated with S powder to generate Mo-doped NiS_(2)(np-NiMo-S)for OER(1.544V vs.RHE at 50mA/cm^(2))and SOR(0.364 V vs.RHE at 50mA/cm^(2)),while still maintaining the nanostructuring advantages.Moreover,for a two-electrode electrolyzer system with np-NiMo cathode(1M KOH+seawater)coupling np-NiMo-S anode(1mol/L KOH+seawater+1 mol/L Na_(2)S),a remarkably ultra-low cell potential of 0.532 V is acquired at 50mA/cm^(2),which is about 1.015 V below that of normal alkaline seawater splitting.The theory calculations confirmed that the AlNi_(3)/Al_(5)Mo heterostructure within np-NiMo promotes H_(2)O dissociation for excellent HER,while the Mo-dopant of np-NiMo-S lowers energy barriers for the rate-determining step from^(*)S_(4)to^(*)S_(8).This work develops two kinds of NiMo alloy with tremendous prominence for achieving energy-efficient hydrogen production from alkaline seawater and sulfur recycling from sulfion-rich sewage.展开更多
A compound containing[FeFe]‑hydrogenase,[Fe_(2)((SCH_(2))_(2)R)(CO)_(6)](1)(R=4‑{(1H‑benzo[d]imidazol‑1‑yl)methyl}‑anilino),was prepared and thoroughly characterized by infrared spectroscopy,single‑crystal X‑ray diffr...A compound containing[FeFe]‑hydrogenase,[Fe_(2)((SCH_(2))_(2)R)(CO)_(6)](1)(R=4‑{(1H‑benzo[d]imidazol‑1‑yl)methyl}‑anilino),was prepared and thoroughly characterized by infrared spectroscopy,single‑crystal X‑ray diffraction,and density functional theory calculations.Its performance as a photocatalyst for hydrogen production via water splitting was evaluated under simulated sunlight.Within 3 h,the amount of H_(2)produced was 386.5μmol,achieving a catalytic efficiency of 25.26μmol·mg^(-1)·h^(-1)and a turnover number(TON)of 0.45.CCDC:2457448.展开更多
Clean hydrogen(H_(2))is highly desirable for the sustainable development of society in the era of carbon neutrality.However,the current capability of water electrolysis and steam methane(CH_(4))reforming to produce gr...Clean hydrogen(H_(2))is highly desirable for the sustainable development of society in the era of carbon neutrality.However,the current capability of water electrolysis and steam methane(CH_(4))reforming to produce green and blue H_(2)is very limited,mainly due to the high production cost,difficult scale-up technology,or operational risk.Here,we propose the direct catalytic decomposition of diesel using a nano-Fe-based catalyst to produce the so-called“jadeite H_(2),”while simultaneously fixing the carbon from the diesel in the form of carbon nanotubes(CNTs).Efforts are made to understand the suppression mechanism of the CH_(4) byproduct,such as by tuning the catalyst type,space velocity,and reaction time.The optimal green index(GI)—that is,the molar ratio of H_(2)/carbon in a gaseous state—of the proposed technology exceeds 42,which is far higher than those of any previously reported chemical vapor deposition(CVD)method.Moreover,the carbon footprint(CFP)of the proposed technology is far lower than those of grey H_(2),blue H_(2),and other dehydrogenation technologies.Compared with most of the technologies mentioned above,the energy consumption(per mole of H_(2))and reactor amplification of the proposed technology validate its high efficiency and great practical feasibility.展开更多
This study examines the feasibility and prospects of integrating marine renewable energy(MRE)with green hydrogen production in Indonesia.As global energy demand increases and the environmental impacts of fossil fuels ...This study examines the feasibility and prospects of integrating marine renewable energy(MRE)with green hydrogen production in Indonesia.As global energy demand increases and the environmental impacts of fossil fuels become more pronounced,the search for sustainable alternatives intensifies.Indonesia,with its extensive maritime resources,presents a unique opportunity to harness tidal wave and offshore wind energy for green hydrogen production from seawater.This research explores various electrolysis methods,particularly those that eliminate the need for desalination,thereby enhancing efficiency and reducing costs.The findings indicate that advanced electrolysis techniques can significantly lower energy and production costs while maintaining environmental sustainability by avoiding harmful chemicals and ensuring minimal ecological footprints.Moreover,the utilization of Indonesia’s extensive marine resources can foster energy independence,boost economic growth,and lower carbon emissions,which highlights the need for ongoing research and optimization to improve the economic and environmental feasibility of these technologies.This review article provides an in-depth analysis of the potential for MRE and green hydrogen production in Indonesia,outlining a viable path toward sustainable energy development.展开更多
Integrating the photovoltaic/thermal(PV/T)system in green hydrogen production is an improvement in sustainable energy technologies.In PV/T systems,solar energy is converted into electricity and thermal energy simultan...Integrating the photovoltaic/thermal(PV/T)system in green hydrogen production is an improvement in sustainable energy technologies.In PV/T systems,solar energy is converted into electricity and thermal energy simultaneously using hot water or air together with electricity.This dual use saves a significant amount of energy and officially fights greenhouse gases.Different cooling techniques have been proposed in the literature for improving the overall performance of the PV/T systems;employing different types of agents including nanofluids and phase change materials.Hydrogen is the lightest and most abundant element in the universe and has later turned into a flexible energy carrier for transportation and other industrial applications.Issues,including the processes of Hydrogen manufacturing,preservation as well as some risks act as barriers.This paper provides an analysis of several recent publications on the efficiency of using PV/T technology in the process of green hydrogen production and indicates the potential for its increased efficiency as compared to conventional systems that rely on fossil fuels.Due to the effective integration of solar energy,the PV/T system can play an important role in the reduction of the levelized cost of hydrogen(LCOH)and hence play an important part in reducing the economic calculations of the decarbonized energy system.展开更多
To address the global energy shortage,hydrogen production as a green energy source has become one of the most prominent research topics over the past decade.Novel and promising ferroelectric materials,exhibiting uniqu...To address the global energy shortage,hydrogen production as a green energy source has become one of the most prominent research topics over the past decade.Novel and promising ferroelectric materials,exhibiting unique spontaneous polarization capabilities,have shown great potential in the field of photocatalytic hydrogen evolution.Among these materials,perovskites represent a significant group of ferroelectrics,possessing both excellent ferroelectric properties and photocatalytic performance.By focusing on perovskites,we analyze the advantages of their built-in electric field for photocatalytic hydrogen evolution,integrating the domain wall structures of ferroelectrics.Furthermore,we summarize how to fully exploit the unique characteristics of ferroelectrics and highlight recent advancements in their application to photocatalytic hydrogen evolution.展开更多
CO_(2)-free H_(2)refers to H_(2)production process without CO_(2)emission,which is a promising clean energy in the future.Catalytic decomposition of methane(CDM)is a competitive technology to produce CO_(2)-free H2 wi...CO_(2)-free H_(2)refers to H_(2)production process without CO_(2)emission,which is a promising clean energy in the future.Catalytic decomposition of methane(CDM)is a competitive technology to produce CO_(2)-free H2 with large-scale.However,CDM reaction is highly endothermic and is kinetically and thermodynamically unfavorable,which typically requires a harsh reaction temperature above 800℃.In this work,solar-driven photothermal catalytic decomposition of methane was firstly introduced to produce CO_(2)-free H_(2)relying solely on solar energy as the driving force.A high H_(2)yield of 204.6 mmol g^(–1)h^(–1)was observed over Ni-CeO2 interface under photothermal conditions,along with above 87%reduction in the apparent activation energy(11.2 vs.87.3 kJ mol^(–1))when comparing with the traditional thermal catalysis.Further studies suggested that Ni/CeO_(2)catalyst enhanced optical absorption in visible-infrared region to ensure the heat energy for methane decomposition.The generated electrons and holes participated in the redox process of photo-driven CDM reaction with enhanced separation ability of hot carriers excited by ultraviolet-visible light,which lowered activation energy and improved the photothermal catalytic activity.This work provides a promising photothermal catalytic strategy to produce CO_(2)-free H^(2)under mild conditions.展开更多
In response to the urgent global need to address climate change,reduce emissions,and ensure energy security,hydrogen plays a crucial role in the global energy transitio n.However,traditional hydrogen production method...In response to the urgent global need to address climate change,reduce emissions,and ensure energy security,hydrogen plays a crucial role in the global energy transitio n.However,traditional hydrogen production methods,such as fossil fuel-based steam reforming and water electrolysis,face significant environmental and economic challenges.As an abundant renewable resource,biomass has attracted much attention for hydrogen production technology,particularly sorption-enhanced steam reforming(SESR).This technology combines the principles of chemical equilibrium and sorption to capture CO_(2) using solid sorbents,thereby enhancing the efficiency and purity of hydrogen production from biomass-derived syngas.It offers advantages such as reduced costs,lower energy consumption,decreased emissions,and cu stomization for specific applications.Although SESR technology has demonstrated excellent hydrogen production performance,existing reviews mainly focus on model compounds and still lack critical analysis of its performance in real biomass application scenarios.This review provides a critical summary of the research progress of biomass feedstocks and model compounds SESR for hydrogen production,detailing the effects of feedstock characteristics,temperature,steam ratio,CO_(2) sorbent(CaO,alkali metal ceramics,and hydrotalcite),and catalysts on gas yield.In addition,it further emphasizes the research progress of advanced sorption-catalysis bifunctional composite materials and discusses the coupling application of SESR technology with other processes.The review concludes by highlighting the outstanding challenges of SESR technology and focusing on future research directions,aiming to provide theoretical support and insights for the further development of sorption-enhanced biomass hydrogen production technology.展开更多
Photocatalytic production of hydrogen peroxide(H_(2)O_(2))presents a promising strategy for environmental remediation and energy production.However,achieving clean and efficient H_(2)O_(2) production under ambient con...Photocatalytic production of hydrogen peroxide(H_(2)O_(2))presents a promising strategy for environmental remediation and energy production.However,achieving clean and efficient H_(2)O_(2) production under ambient conditions without organic sacrificial agents remains challenging.Enhancing the low crystallinity of covalent organic frameworks(COFs)can promote the separation and transmission of photo-generated carriers,thereby boosting their photocatalytic performance.Herein,we introduce a novel synthetic approach by substituting traditional acetic acid catalysts with organic base catalysts to enhance the crystallinity of β-ketoenamine-linked COF,TpBD-COF.Compared to TpBD-COF-A synthesized using acetic acid catalysts,TpBD-COF-B,synthesized with organic base catalysts,exhibited advancements including increased absorption intensity in the visible spectrum,reduced photoluminescence intensity,enhanced photo-generated carrier separation performance,and a 2.1-fold increase in photocatalytic H_(2)O_(2) production.Under visible light irradiation,TpBDCOF-B achieved a photocatalytic H_(2)O_(2) production rate of 533μmol/h/g using only air and water,without the need for organic sacrificial agents.Furthermore,TpBD-COF-B also exhibited good performance in long-term catalytic production experiments,tests with actual water bodies,and cyclic usage experiments.This study offers a strategy for enhancing the crystallinity of COFs to improve their photocatalytic activity,with promising applications in clean energy production and environmental remediation.展开更多
Hydrogen peroxide(H_(2)O_(2))is a versatile compound with widespread applications in various industries.In addition,it has attracted inte rest as a potential energy carrier due to its high energy density and ability t...Hydrogen peroxide(H_(2)O_(2))is a versatile compound with widespread applications in various industries.In addition,it has attracted inte rest as a potential energy carrier due to its high energy density and ability to release oxygen upon decomposition.The development of photocatalytic technology has enabled sustainable production of H_(2)O_(2).Various structural materials,including organic molecules,polymers,and metal coordination compounds,have been synthesized for investigating photocatalytic H_(2)O_(2)production.Rare earth materials,in particular,are of interest due to their adjustable porosity and controllable metal active sites,making them valuable for research in this field.These materials have excellent photoelectric properties,making them promise for the photocatalytic synthesis of H_(2)O_(2).Despite limited reports on systematic reviews of photocatalytic H_(2)O_(2)production using rare earth materials,this study introduces the principles and advancements in this area.It reviews different methods of photocatalytic synthesis of H_(2)O_(2),focusing on rare earth elements.Through comprehensive analysis and systematic studies in the existing literature,a deeper understanding of enhanced photocatalytic performance has been achieved.This research not only contributes to advancing fundamental knowledge but also provides a solid foundation for practical applications.展开更多
Hydrogen energy,as the ultimate clean energy,effectively avoids the greenhouse effect.Chemical looping hydrogen production(CLHP),a versatile energy conversion and production technology,has garnered extensive attention...Hydrogen energy,as the ultimate clean energy,effectively avoids the greenhouse effect.Chemical looping hydrogen production(CLHP),a versatile energy conversion and production technology,has garnered extensive attention.CLHP demands redox catalysts with high oxygen capacity,regulatable reactivity,and structural integrity even under harsh operational conditions.Currently,sintering,agglomeration,and inactivation of redox catalysts during cyclic lattice oxygen release and restoration are challenging,hindering the wide industrialization of the chemical looping(CL)process.Moreover,the precise control of activity and reaction rate of the redox catalysts to flexibly accommodate the demands of various reaction substrates remains unclear.This paper introduces the design of a nano-scaled redox catalyst featuring a unique core-shell structure.By precisely controlling the shell thickness,a series of hierarchical Fe_(2)O_(3)@SiO_(2)redox catalysts were successfully synthesized.Building on this achievement,an in-depth investigation was conducted into the impact of the thickness and spatial structure of the inert support on the stability and mass transfer rate of the redox catalyst,aiming to achieve a perfect balance between these two factors during the CLHP process.A thin shell(70 nm)exhibits excellent cyclic stability,maintaining consistent performance in 30 consecutive redox cycles,while a thicker shell(200 nm)undergoes rapid deactivation due to the formation of a substantial amount of iron silicate.In-situ transmission electron microscopy(TEM)reveals that the SiO_(2)shell effectively restricts the agglomeration of Fe_(2)O_(3).The unique core-shell structure and controllable shell thickness offer novel insights into the flexible design of efficient and durable hierarchical redox catalysts with spatial structure.展开更多
Proton Exchange Membrane Water Electrolyzers(PEMWE)are efficient and sustainable hydrogen production devices.This article analyzes their static and dynamic electrical models integrated with degradation mechanisms.Stat...Proton Exchange Membrane Water Electrolyzers(PEMWE)are efficient and sustainable hydrogen production devices.This article analyzes their static and dynamic electrical models integrated with degradation mechanisms.Static models reveal steady-state behavior,while dynamic models capture transient responses to input variations.The developed modeling approach combines the activation and diffusion phenomena,resulting in a novel PEMWE model that closely reflects real-world conditions and enables fast simulations.The electrical model is integrated with the aging model through two key ratios,surface degradation ratio and membrane degradation ratio,which characterize degradation mechanisms affecting electrode and membrane performance.The linear model using second-order Taylor approximation enables the development of a diagnosis approach that can contribute to estimating the remaining useful life of PEMWEs.By associating aging models with electrical models through the proposed ratios,a deeper understanding is achieved regarding how degra-dation phenomena evolve and influence electrolyzer efficiency and durability.The integrated framework enables predictive maintenance strategies,making it valuable for industrial hydrogen production applications.展开更多
Oxysulfide semiconductors are promising photocatalysts for visible light-driven water splitting.For a widely studied narrow-bandgap Sm_(2)Ti_(2)O_(5)S_(2)(STOS),limited bulk charge separation and slow surface reaction...Oxysulfide semiconductors are promising photocatalysts for visible light-driven water splitting.For a widely studied narrow-bandgap Sm_(2)Ti_(2)O_(5)S_(2)(STOS),limited bulk charge separation and slow surface reaction heavily restrict its photocatalytic performance.Here,well-crystallized STOS oxysulfide nanosheets,synthesized by a flux-assisted solid-state reaction,were proved to show prominent facet-oriented charge transport property,in which photogenerated electrons migrated to{101}planes and holes to{001}planes of each particle.Hydrogen evolution cocatalysts were therefore precisely positioned on the electron-rich facets to boost the water reduction reaction.In particular,in-situ formation of a Ptshell@Ircore core-shell structure on the electron-rich{101}facets and an IrO_(2) on the hole-accumulated{001}facets greatly assisted the sacrificial photocatalytic H_(2) production over STOS,resulting in an apparent quantum yield as high as 35.9%at 420 nm.By using the highly-active STOS as H_(2) evolution photocatalyst,a Mo:BiVO_(4) as oxygen evolution photocatalyst,and a[Co(bpy)_(3)]^(2+/3+)as redox shuttle,a Z-Scheme overall water splitting system was constructed to achieve a solar-to-hydrogen conversion efficiency of 0.175%.This work not only elucidates the facet-dependent charge transfer mechanism on STOS but also proposes an ideal strategy for enhancing its photocatalytic performance.展开更多
基金supported by the Strategic Priority Research Program of the Chinese Academy of Sciences(No.XDA0400000)the Youth Innovation Promotion Association of the Chinese Academy of Sciences(No.2021253)+1 种基金the Major Science and Technology Projects of China National Offshore Oil Corporation Limited during the 14th Five Year Plan(No.KJGG-2022-12-CCUS-030500)the Photon Science Center for Carbon Neutrality of Chinese Academy of Science.
文摘When the operating temperature of a solid oxide electrolysis cell(SOEC)is lower than the outlet temperature of a nuclear reactor,the reactor can be directly coupled with the SOEC as a high-temperature heat source.However,the key to the efficiency and return on investment of this hybrid energy system lies in the expected lifetime of the SOEC.This study assessed Ni-YSZ|YSZ|GDC|LSC fuel electrode support cells’long-term stability during electrolysis at 650℃with a current density of−0.5Acm^(−2)over 1818 h.The average voltage degradation rate of 2.63%kh^(−1)unfolded in two phases:an initial rapid decay(90 to 1120 h at 3.58%kh^(−1))and a stable decay(1120 to 1818 h at 2.14%kh^(−1)),emphasizing SOECs’probability coupling with nuclear reactors at 650℃.Post-1818-hour electrolysis revealed nickel particle formation associated with Ni(OH)_(x)diffusion and re-deposition,alongside a strontium-containing layer causing interface cracking.Despite minimal strontium segregation in the EDS,XPS data indicated surface segregation of Sr.This study provides crucial insights into prolonged SOEC operation,highlighting both its potential and challenges.
基金supported by Natural Science Foundation of Shanghai,under the Shanghai Action Plan for Science,Technology and Innovation(22ZR1464800).
文摘Driven by the global energy transition and carbon neutrality targets,alkaline water electrolysis has emerged as a key technology for coupling variable renewable generation with clean hydrogen production,offering considerable potential for absorbing surplus power and enhancing grid flexibility.However,conventional control architectures typically treat the power converter and electrolyzer as independent units,neglecting their dynamic interactions and thereby limiting overall system performance under practical operating conditions.This review critically examines existing control approaches,ranging from classical proportional-integral schemes to model predictive control,fuzzy-logic algorithms,and data-driven methods,evaluating their effectiveness in managing dynamic response,multivariable coupling,and operational constraints as well as their inherent limitations.Attention is then focused on the performance requirements of the hydrogen-production converter,including current ripple suppression,rapid transient response,adaptive thermal regulation,and stable power delivery.An integrated co‑control framework is proposed,aligning converter output with electrolyzer demand across steady-state operation,variable renewable input,and emergency shutdown scenarios to achieve higher efficiency,extended equipment lifetime,and enhanced operational safety.Finally,prospects for advancing unified control methodologies are outlined,with emphasis on constraint-aware predictive control,machine-learning-enhanced modeling,and real‑time co‑optimization for future alkaline electrolyzer systems.
基金the funding from the National Natural Science Foundation of China(22275001)the Project of Anhui Provincial Department of Education(2022AH010004,KJ2021ZD0002)。
文摘Electrocatalytic water splitting for green hydrogen is hindered by the slow oxygen evolution reaction(OER).Replacing OER with ethylene glycol oxidation(EGOR)offers an energy-saving route,coproducing valuable chemicals,but requires efficient,stable,and low-cost catalysts.Here,we report a sulfate-doped NiOOH-Ni(OH)_(2)catalyst(denoted S-NiOOH-Ni(OH)_(2)).SO_(4)^(2-)doping significantly boosts intrinsic activity,enabling exceptional EGOR performance(only 1.45 V for~650 mA cm^(-2)).In situ studies reveal that a unique"structural locking"effect stabilizes the highly activeβ-NiOOH phase within the composite,differing from conventional reconstruction.Notably,we successfully scaled up this catalyst to an industrial-scale electrolyzer(anode area:1386 cm^(2))and constructed an integrated electrochemical-conventional chemical coupling system,which stably produced 290 L of hydrogen and kilogram-scale high-purity potassium diformate(KDF)per batch.Techno-economic analysis confirms strong commercial viability,projecting$7.1 million annual profit and a payback period under one year.This work bridges advanced catalyst design to industrial biomass valorization coupled with hydrogen production.
基金supported by National Natural Science Foundation of China(22478076,U25B6005)National Key R&D Program of China(2021YFA1500302)+1 种基金Industrial Joint Fund of Qingyuan Innovation Laboratory(00422001)111 Project(D17005).
文摘The efficient storage and release of H_(2)are pivotal for the advancement of hydrogen energy technologies.Cyclohexane,as a promising liquid organic hydrogen carrier(LOHC),provides a safe and practical solution for H_(2)storage.However,the performance limitations of dehydrogenation catalysts have hindered the rapid development of LOHC technology.In this study,we successfully developed boron-modified Pt/ZrO_(2)catalysts,which exhibit exceptional catalytic performance in cyclohexane dehydrogenation.The optimal boron content is determined to be 0.5 wt.%,with the Pt/0.5B–ZrO_(2)catalyst achieving high turnover frequency(TOF)of 10,627.3 mol_(H_(2))·mol_(Pt)^(−1)·h^(−1)and benzene selectivity of 99%at 295°C.The catalyst also demonstrates H_(2)evolution rate of 908 mmol·g_(Pt)^(−1)·min^(−1)and low deactivation rate of 0.0043 h^(−1).Remarkably,the catalyst displays outstanding stability and regeneration performance,maintaining its activity without significant loss during a 60-h dehydrogenation reaction and retaining a cyclohexane conversion of 77.2%after 10 consecutive cycles.Comprehensive characterization techniques,including XPS,CO-FTIR,NH_(3)-TPD,H_(2)-TPD,Benzene-TPD,and Py-IR,reveals that boron modification reduces the electron density of Pt,generating abundant electron-deficient Pt atoms.These electron-deficient Pt atoms enhance H_(2)adsorption and accelerate benzene desorption,effectively preventing coke formation from deep benzene dehydrogenation,which is responsible for the high catalytic performance of the Pt/0.5B–ZrO_(2)catalyst.These findings offer a valuable strategy for optimizing dehydrogenation catalysts in LOHC technologies,addressing a critical bottleneck in the development of this essential energy storage solution.
基金National Natural Science Foundation of China(No.52476192,No.52106237)Natural Science Foundation of Heilongjiang Province(No.YQ2022E027)。
文摘The transition of hydrogen sourcing from carbon-intensive to water-based methodologies is underway,with renewable energy-powered proton exchange membrane water electrolysis(PEMWE)emerging as the preeminent pathway for hydrogen production.Despite remarkable advancements in this field,confronting the sluggish electrochemical kinetics and inherent high-energy consumption arising from deteriorated mass transport within PEMWE systems remains a formidable obstacle.This impediment stems primarily from the hindered protons mass transfer and the untimely hydrogen bubbles detachment.To address these challenges,we harness the inherent variability of electrical energy and introduce an innovative pulsed dynamic water electrolysis system.Compared to constant voltage electrolysis(hydrogen production rate:51.6 m L h^(-1),energy consumption:5.37 kWh Nm-^(3)H_(2)),this strategy(hydrogen production rate:66 m L h^(-1),energy consumption:3.83 kWh Nm-^(3)H_(2))increases the hydrogen production rate by approximately 27%and reduces the energy consumption by about 28%.Furthermore,we demonstrate the practicality of this system by integrating it with an off-grid photovoltaic(PV)system designed for outdoor operation,successfully driving a hydrogen production current of up to 500 mA under an average voltage of approximately 2 V.The combined results of in-situ characterization and finite element analysis reveal the performance enhancement mechanism:pulsed dynamic electrolysis(PDE)dramatically accelerates the enrichment of protons at the electrode/solution interface and facilitates the release of bubbles on the electrode surface.As such,PDE-enhanced PEMWE represents a synergistic advancement,concurrently enhancing both the hydrogen generation reaction and associated transport processes.This promising technology not only redefines the landscape of electrolysis-based hydrogen production but also holds immense potential for broadening its application across a diverse spectrum of electrocatalytic endeavors.
基金National Key R&D Program of China,Grant/Award Number:2021YFA1500900Basic and Applied Basic Research Foundation of Guangdong Province-Regional Joint Fund Project,Grant/Award Number:2021B1515120024+9 种基金Science Funds of the Education Office of Jiangxi Province,Grant/Award Number:GJJ2201324Science Funds of Jiangxi Province,Grant/Award Numbers:20242BAB25168,20224BAB213018Doctoral Research Start-up Funds of JXSTNU,Grant/Award Number:2022BSQD05China Postdoctoral Science Foundation,Grant/Award Number:2023M741121National Natural Science Foundation of China,Grant/Award Number:22172047Provincial Natural Science Foundation of Hunan,Grant/Award Number:2021JJ30089Shenzhen Science and Technology Program,Grant/Award Number:JCYJ20210324122209025Changsha Municipal Natural Science Foundation,Grant/Award Number:kq2107008Hunan Province of Huxiang Talent project,Grant/Award Number:2023rc3118Natural Science Foundation of Hunan Province,Grant/Award Number:2022JJ10006.
文摘Hydrogen energy from electrocatalysis driven by sustainable energy has emerged as a solution against the background of carbon neutrality.Proton exchange membrane(PEM)-based electrocatalytic systems represent a promising technology for hydrogen production,which is equipped to combine efficiently with intermittent electricity from renewable energy sources.In this review,PEM-based electrocatalytic systems for H2 production are summarized systematically from low to high operating temperature systems.When the operating temperature is below 130℃,the representative device is a PEM water electrolyzer;its core components and respective functions,research status,and design strategies of key materials especially in electrocatalysts are presented and discussed.However,strong acidity,highly oxidative operating conditions,and the sluggish kinetics of the anode reaction of PEM water electrolyzers have limited their further development and shifted our attention to higher operating temperature PEM systems.Increasing the temperature of PEM-based electrocatalytic systems can cause an increase in current density,accelerate reaction kinetics and gas transport and reduce the ohmic value,activation losses,ΔGH*,and power consumption.Moreover,further increasing the operating temperature(120-300℃)of PEM-based devices endows various hydrogen carriers(e.g.,methanol,ethanol,and ammonia)with electrolysis,offering a new opportunity to produce hydrogen using PEM-based electrocatalytic systems.Finally,several future directions and prospects for developing PEM-based electrocatalytic systems for H_(2) production are proposed through devoting more efforts to the key components of devices and reduction of costs.
基金supported by the National Natural Science Foundation of China(Grant Nos.22162025,22168040)the Youth Innovation Team of Shaanxi Universities,the Open and Innovation Fund of Hubei Three Gorges Laboratory(SK232001)the Regional Innovation Capability Leading Program of Shaanxi(2022QFY07-03,2022QFY07-06).
文摘Electrocatalytic urea wastewater treatment technology has emerged as a promising method for environmental remediation.However,the realization of highly efficient and scalable electrocatalytic urea wastewater treatment(SEUWT)is still an enormous challenge.Herein,through regulating the adsorption behavior of urea functional groups,the efficient SEUWT coupled hydrogen production is realized in anion exchange membrane water electrolyzer(AEMWE).Density functional theory calculations indicate that self-driven electron transfer at the heterogeneous interface(NiO/Co_(3)O_(4))can induce charge redistribution,resulting in electron-rich NiO and electron-deficient Co_(3)O_(4),which are superior to adsorbing C=O(electron-withdrawing group)and–NH_(2)(electron-donating group),respectively,regulating the adsorption behavior of urea molecule and accelerating the reaction kinetics of urea oxidation.This viewpoint is further verified by temperature-programmed desorption experiments.The SEUWT coupled hydrogen production in AEMWE assembled with NiO/Co_(3)O_(4)(anode)and NiCoP(cathode)can continuously treat urea wastewater at an initial current density of 600 mA cm^(-2),with the average urea treatment efficiency about 53%.Compared with overall water splitting,the H_(2) production rate(8.33 mmol s^(-1))increases by approximately 3.5 times.This work provides a cost-effective strategy for scalable purifying urea-rich wastewater and energy-saving hydrogen production.
基金financially supported by the Guangxi Natural Science Fund for Distinguished Young Scholars(No.2024GXNSFFA010008)the Natural Science Foundation of Jilin Province of China(No.20240101098JC)the National Natural Science Foundation of China(No.22469002)。
文摘Establishing an energy-saving and affordable hydrogen production route from infinite seawater presents a promising strategy for achieving carbon neutrality and low-carbon development.Compared with the kinetically sluggish oxygen evolution reaction(OER),the thermodynamically advantageous sulfion oxidation reaction(SOR)enables the S^(2-)pollutants recovery while reducing the energy input of water electrolysis.Here,a nanoporous NiMo alloy ligament(np-NiMo)with AlNi_(3)/Al_(5)Mo heterostructure was prepared for hydrogen evolution reaction(HER,-0.134V versus reversible hydrogen electrode(vs.RHE)at 50mA/cm^(2)),which needs an Al_(89)Ni_(10)Mo_(1)as a precursor and dealloying operation.Further,the np-NiMo alloy was thermal-treated with S powder to generate Mo-doped NiS_(2)(np-NiMo-S)for OER(1.544V vs.RHE at 50mA/cm^(2))and SOR(0.364 V vs.RHE at 50mA/cm^(2)),while still maintaining the nanostructuring advantages.Moreover,for a two-electrode electrolyzer system with np-NiMo cathode(1M KOH+seawater)coupling np-NiMo-S anode(1mol/L KOH+seawater+1 mol/L Na_(2)S),a remarkably ultra-low cell potential of 0.532 V is acquired at 50mA/cm^(2),which is about 1.015 V below that of normal alkaline seawater splitting.The theory calculations confirmed that the AlNi_(3)/Al_(5)Mo heterostructure within np-NiMo promotes H_(2)O dissociation for excellent HER,while the Mo-dopant of np-NiMo-S lowers energy barriers for the rate-determining step from^(*)S_(4)to^(*)S_(8).This work develops two kinds of NiMo alloy with tremendous prominence for achieving energy-efficient hydrogen production from alkaline seawater and sulfur recycling from sulfion-rich sewage.
文摘A compound containing[FeFe]‑hydrogenase,[Fe_(2)((SCH_(2))_(2)R)(CO)_(6)](1)(R=4‑{(1H‑benzo[d]imidazol‑1‑yl)methyl}‑anilino),was prepared and thoroughly characterized by infrared spectroscopy,single‑crystal X‑ray diffraction,and density functional theory calculations.Its performance as a photocatalyst for hydrogen production via water splitting was evaluated under simulated sunlight.Within 3 h,the amount of H_(2)produced was 386.5μmol,achieving a catalytic efficiency of 25.26μmol·mg^(-1)·h^(-1)and a turnover number(TON)of 0.45.CCDC:2457448.
基金supported by the National Natural Science Foundation of China(22109085 and 21975142)the Tsinghua–Sinopec joint project(123068 and 20232930013).
文摘Clean hydrogen(H_(2))is highly desirable for the sustainable development of society in the era of carbon neutrality.However,the current capability of water electrolysis and steam methane(CH_(4))reforming to produce green and blue H_(2)is very limited,mainly due to the high production cost,difficult scale-up technology,or operational risk.Here,we propose the direct catalytic decomposition of diesel using a nano-Fe-based catalyst to produce the so-called“jadeite H_(2),”while simultaneously fixing the carbon from the diesel in the form of carbon nanotubes(CNTs).Efforts are made to understand the suppression mechanism of the CH_(4) byproduct,such as by tuning the catalyst type,space velocity,and reaction time.The optimal green index(GI)—that is,the molar ratio of H_(2)/carbon in a gaseous state—of the proposed technology exceeds 42,which is far higher than those of any previously reported chemical vapor deposition(CVD)method.Moreover,the carbon footprint(CFP)of the proposed technology is far lower than those of grey H_(2),blue H_(2),and other dehydrogenation technologies.Compared with most of the technologies mentioned above,the energy consumption(per mole of H_(2))and reactor amplification of the proposed technology validate its high efficiency and great practical feasibility.
基金Supported by The Indonesia Endowment Funds for Education or Lembaga Pengelola Pendidikan(LPDP)Ministry of Finance with scholarship contracts 0000559/TRP/M/19/lpdp2023.
文摘This study examines the feasibility and prospects of integrating marine renewable energy(MRE)with green hydrogen production in Indonesia.As global energy demand increases and the environmental impacts of fossil fuels become more pronounced,the search for sustainable alternatives intensifies.Indonesia,with its extensive maritime resources,presents a unique opportunity to harness tidal wave and offshore wind energy for green hydrogen production from seawater.This research explores various electrolysis methods,particularly those that eliminate the need for desalination,thereby enhancing efficiency and reducing costs.The findings indicate that advanced electrolysis techniques can significantly lower energy and production costs while maintaining environmental sustainability by avoiding harmful chemicals and ensuring minimal ecological footprints.Moreover,the utilization of Indonesia’s extensive marine resources can foster energy independence,boost economic growth,and lower carbon emissions,which highlights the need for ongoing research and optimization to improve the economic and environmental feasibility of these technologies.This review article provides an in-depth analysis of the potential for MRE and green hydrogen production in Indonesia,outlining a viable path toward sustainable energy development.
基金funding support from Arabian Gulf University to cover any necessary publication fees.
文摘Integrating the photovoltaic/thermal(PV/T)system in green hydrogen production is an improvement in sustainable energy technologies.In PV/T systems,solar energy is converted into electricity and thermal energy simultaneously using hot water or air together with electricity.This dual use saves a significant amount of energy and officially fights greenhouse gases.Different cooling techniques have been proposed in the literature for improving the overall performance of the PV/T systems;employing different types of agents including nanofluids and phase change materials.Hydrogen is the lightest and most abundant element in the universe and has later turned into a flexible energy carrier for transportation and other industrial applications.Issues,including the processes of Hydrogen manufacturing,preservation as well as some risks act as barriers.This paper provides an analysis of several recent publications on the efficiency of using PV/T technology in the process of green hydrogen production and indicates the potential for its increased efficiency as compared to conventional systems that rely on fossil fuels.Due to the effective integration of solar energy,the PV/T system can play an important role in the reduction of the levelized cost of hydrogen(LCOH)and hence play an important part in reducing the economic calculations of the decarbonized energy system.
基金supports from the Scientific Research Foundation of Hunan Provincial Education Department(21A0188,24C0149)the National Natural Science Foundation of China(52400202)+3 种基金Engineering and Technical Center Open Fund of Hunan Provincial Environmental Protection for River-Lake Dredging Pollution Control(EPD202104)Natural Science Foundation of Hunan Province(2023JJ40028,2024JJ6058)Natural Science Foundation of Changsha City(kq2208232)Natural Science Foundation of Hunan Province(2023JJ40033).
文摘To address the global energy shortage,hydrogen production as a green energy source has become one of the most prominent research topics over the past decade.Novel and promising ferroelectric materials,exhibiting unique spontaneous polarization capabilities,have shown great potential in the field of photocatalytic hydrogen evolution.Among these materials,perovskites represent a significant group of ferroelectrics,possessing both excellent ferroelectric properties and photocatalytic performance.By focusing on perovskites,we analyze the advantages of their built-in electric field for photocatalytic hydrogen evolution,integrating the domain wall structures of ferroelectrics.Furthermore,we summarize how to fully exploit the unique characteristics of ferroelectrics and highlight recent advancements in their application to photocatalytic hydrogen evolution.
文摘CO_(2)-free H_(2)refers to H_(2)production process without CO_(2)emission,which is a promising clean energy in the future.Catalytic decomposition of methane(CDM)is a competitive technology to produce CO_(2)-free H2 with large-scale.However,CDM reaction is highly endothermic and is kinetically and thermodynamically unfavorable,which typically requires a harsh reaction temperature above 800℃.In this work,solar-driven photothermal catalytic decomposition of methane was firstly introduced to produce CO_(2)-free H_(2)relying solely on solar energy as the driving force.A high H_(2)yield of 204.6 mmol g^(–1)h^(–1)was observed over Ni-CeO2 interface under photothermal conditions,along with above 87%reduction in the apparent activation energy(11.2 vs.87.3 kJ mol^(–1))when comparing with the traditional thermal catalysis.Further studies suggested that Ni/CeO_(2)catalyst enhanced optical absorption in visible-infrared region to ensure the heat energy for methane decomposition.The generated electrons and holes participated in the redox process of photo-driven CDM reaction with enhanced separation ability of hot carriers excited by ultraviolet-visible light,which lowered activation energy and improved the photothermal catalytic activity.This work provides a promising photothermal catalytic strategy to produce CO_(2)-free H^(2)under mild conditions.
基金supported by the National Natural Science Foundation of China(No.52276193)。
文摘In response to the urgent global need to address climate change,reduce emissions,and ensure energy security,hydrogen plays a crucial role in the global energy transitio n.However,traditional hydrogen production methods,such as fossil fuel-based steam reforming and water electrolysis,face significant environmental and economic challenges.As an abundant renewable resource,biomass has attracted much attention for hydrogen production technology,particularly sorption-enhanced steam reforming(SESR).This technology combines the principles of chemical equilibrium and sorption to capture CO_(2) using solid sorbents,thereby enhancing the efficiency and purity of hydrogen production from biomass-derived syngas.It offers advantages such as reduced costs,lower energy consumption,decreased emissions,and cu stomization for specific applications.Although SESR technology has demonstrated excellent hydrogen production performance,existing reviews mainly focus on model compounds and still lack critical analysis of its performance in real biomass application scenarios.This review provides a critical summary of the research progress of biomass feedstocks and model compounds SESR for hydrogen production,detailing the effects of feedstock characteristics,temperature,steam ratio,CO_(2) sorbent(CaO,alkali metal ceramics,and hydrotalcite),and catalysts on gas yield.In addition,it further emphasizes the research progress of advanced sorption-catalysis bifunctional composite materials and discusses the coupling application of SESR technology with other processes.The review concludes by highlighting the outstanding challenges of SESR technology and focusing on future research directions,aiming to provide theoretical support and insights for the further development of sorption-enhanced biomass hydrogen production technology.
基金jointly supported by the Strategic Priority Research Program of the Chinese Academy of Sciences(No.XDB0750200)the National Key Research and Development Program of China(No.2023YFC3706600)the National Natural Science Foundation of China(Nos.22225605 and 22193051).
文摘Photocatalytic production of hydrogen peroxide(H_(2)O_(2))presents a promising strategy for environmental remediation and energy production.However,achieving clean and efficient H_(2)O_(2) production under ambient conditions without organic sacrificial agents remains challenging.Enhancing the low crystallinity of covalent organic frameworks(COFs)can promote the separation and transmission of photo-generated carriers,thereby boosting their photocatalytic performance.Herein,we introduce a novel synthetic approach by substituting traditional acetic acid catalysts with organic base catalysts to enhance the crystallinity of β-ketoenamine-linked COF,TpBD-COF.Compared to TpBD-COF-A synthesized using acetic acid catalysts,TpBD-COF-B,synthesized with organic base catalysts,exhibited advancements including increased absorption intensity in the visible spectrum,reduced photoluminescence intensity,enhanced photo-generated carrier separation performance,and a 2.1-fold increase in photocatalytic H_(2)O_(2) production.Under visible light irradiation,TpBDCOF-B achieved a photocatalytic H_(2)O_(2) production rate of 533μmol/h/g using only air and water,without the need for organic sacrificial agents.Furthermore,TpBD-COF-B also exhibited good performance in long-term catalytic production experiments,tests with actual water bodies,and cyclic usage experiments.This study offers a strategy for enhancing the crystallinity of COFs to improve their photocatalytic activity,with promising applications in clean energy production and environmental remediation.
基金Project supported by the National Natural Science Foundation of China(22205084,42307566)the China Postdoctoral Science Foundation(2023M741039,2023M742199)+1 种基金the Science and Technology Project of Henan Province(232102321035)the State Key Laboratory of Efficient Utilization for Low Grade Phosphate Rock and Its Associated Resources(WFKF(2023)013)。
文摘Hydrogen peroxide(H_(2)O_(2))is a versatile compound with widespread applications in various industries.In addition,it has attracted inte rest as a potential energy carrier due to its high energy density and ability to release oxygen upon decomposition.The development of photocatalytic technology has enabled sustainable production of H_(2)O_(2).Various structural materials,including organic molecules,polymers,and metal coordination compounds,have been synthesized for investigating photocatalytic H_(2)O_(2)production.Rare earth materials,in particular,are of interest due to their adjustable porosity and controllable metal active sites,making them valuable for research in this field.These materials have excellent photoelectric properties,making them promise for the photocatalytic synthesis of H_(2)O_(2).Despite limited reports on systematic reviews of photocatalytic H_(2)O_(2)production using rare earth materials,this study introduces the principles and advancements in this area.It reviews different methods of photocatalytic synthesis of H_(2)O_(2),focusing on rare earth elements.Through comprehensive analysis and systematic studies in the existing literature,a deeper understanding of enhanced photocatalytic performance has been achieved.This research not only contributes to advancing fundamental knowledge but also provides a solid foundation for practical applications.
基金financial support from the National Natural Science Foundation of China(52076209,22179027,22469006)the Foundation and Applied Foundation Research of Guangdong Province(2022B1515020045)the Heilongjiang Key Research and Development Project of China(JD22A026)。
文摘Hydrogen energy,as the ultimate clean energy,effectively avoids the greenhouse effect.Chemical looping hydrogen production(CLHP),a versatile energy conversion and production technology,has garnered extensive attention.CLHP demands redox catalysts with high oxygen capacity,regulatable reactivity,and structural integrity even under harsh operational conditions.Currently,sintering,agglomeration,and inactivation of redox catalysts during cyclic lattice oxygen release and restoration are challenging,hindering the wide industrialization of the chemical looping(CL)process.Moreover,the precise control of activity and reaction rate of the redox catalysts to flexibly accommodate the demands of various reaction substrates remains unclear.This paper introduces the design of a nano-scaled redox catalyst featuring a unique core-shell structure.By precisely controlling the shell thickness,a series of hierarchical Fe_(2)O_(3)@SiO_(2)redox catalysts were successfully synthesized.Building on this achievement,an in-depth investigation was conducted into the impact of the thickness and spatial structure of the inert support on the stability and mass transfer rate of the redox catalyst,aiming to achieve a perfect balance between these two factors during the CLHP process.A thin shell(70 nm)exhibits excellent cyclic stability,maintaining consistent performance in 30 consecutive redox cycles,while a thicker shell(200 nm)undergoes rapid deactivation due to the formation of a substantial amount of iron silicate.In-situ transmission electron microscopy(TEM)reveals that the SiO_(2)shell effectively restricts the agglomeration of Fe_(2)O_(3).The unique core-shell structure and controllable shell thickness offer novel insights into the flexible design of efficient and durable hierarchical redox catalysts with spatial structure.
文摘Proton Exchange Membrane Water Electrolyzers(PEMWE)are efficient and sustainable hydrogen production devices.This article analyzes their static and dynamic electrical models integrated with degradation mechanisms.Static models reveal steady-state behavior,while dynamic models capture transient responses to input variations.The developed modeling approach combines the activation and diffusion phenomena,resulting in a novel PEMWE model that closely reflects real-world conditions and enables fast simulations.The electrical model is integrated with the aging model through two key ratios,surface degradation ratio and membrane degradation ratio,which characterize degradation mechanisms affecting electrode and membrane performance.The linear model using second-order Taylor approximation enables the development of a diagnosis approach that can contribute to estimating the remaining useful life of PEMWEs.By associating aging models with electrical models through the proposed ratios,a deeper understanding is achieved regarding how degra-dation phenomena evolve and influence electrolyzer efficiency and durability.The integrated framework enables predictive maintenance strategies,making it valuable for industrial hydrogen production applications.
文摘Oxysulfide semiconductors are promising photocatalysts for visible light-driven water splitting.For a widely studied narrow-bandgap Sm_(2)Ti_(2)O_(5)S_(2)(STOS),limited bulk charge separation and slow surface reaction heavily restrict its photocatalytic performance.Here,well-crystallized STOS oxysulfide nanosheets,synthesized by a flux-assisted solid-state reaction,were proved to show prominent facet-oriented charge transport property,in which photogenerated electrons migrated to{101}planes and holes to{001}planes of each particle.Hydrogen evolution cocatalysts were therefore precisely positioned on the electron-rich facets to boost the water reduction reaction.In particular,in-situ formation of a Ptshell@Ircore core-shell structure on the electron-rich{101}facets and an IrO_(2) on the hole-accumulated{001}facets greatly assisted the sacrificial photocatalytic H_(2) production over STOS,resulting in an apparent quantum yield as high as 35.9%at 420 nm.By using the highly-active STOS as H_(2) evolution photocatalyst,a Mo:BiVO_(4) as oxygen evolution photocatalyst,and a[Co(bpy)_(3)]^(2+/3+)as redox shuttle,a Z-Scheme overall water splitting system was constructed to achieve a solar-to-hydrogen conversion efficiency of 0.175%.This work not only elucidates the facet-dependent charge transfer mechanism on STOS but also proposes an ideal strategy for enhancing its photocatalytic performance.
