A CuPc/SiO2 sample is fabricated. Its morphology is characterized by atomic force microscopy, and the electron states are investigated by X-ray photoelectron spectroscopy. In order to investigate these spectra in deta...A CuPc/SiO2 sample is fabricated. Its morphology is characterized by atomic force microscopy, and the electron states are investigated by X-ray photoelectron spectroscopy. In order to investigate these spectra in detail, all of these spectra are normalized to the height of the most intense peak,and each component is fitted with a single Gaussian function. Analysis shows that the O element has great bearing on the electron states and that SiO2 layers produced by spurting technology are better than those produced by oxidation technology.展开更多
CeO_(2) based semiconductor are widely used in solar-driven photothermal catalytic dry reforming of methane(DRM)reaction,but still suffer from low activity and low light utilization efficiency.This study developed gra...CeO_(2) based semiconductor are widely used in solar-driven photothermal catalytic dry reforming of methane(DRM)reaction,but still suffer from low activity and low light utilization efficiency.This study developed graphite-CeO_(2) interfaces to enhance solar-driven photothermal catalytic DRM.Compared with carbon nanotubes-modified CeO_(2)(CeO_(2)-CNT),graphite-modified CeO_(2)(CeO_(2)-GRA)constructed graphite-CeO_(2) interfaces with distortion in CeO_(2),leading to the formation abundant oxygen vacancies.These graphite-CeO_(2) interfaces with oxygen vacancies enhanced optical absorption and promoted the generation and separation of photogenerated carriers.The high endothermic capacity of graphite elevated the catalyst surface temperature from 592.1−691.3℃,boosting light-to-thermal conversion.The synergy between photogenerated carriers and localized heat enabled Ni/CeO_(2)-GRA to achieve a CO production rate of 9985.6 mmol/(g·h)(vs 7192.4 mmol/(g·h)for Ni/CeO_(2))and a light-to-fuel efficiency of 21.8%(vs 13.8%for Ni/CeO_(2)).This work provides insights for designing graphite-semiconductor interfaces to advance photothermal catalytic efficiency.展开更多
Metal-carbon dioxide(CO_(2))batteries hold great promise for reducing greenhouse gas emissions and are regarded as one of the most promising energy storage techniques due to their efficiency advantages in CO_(2)recove...Metal-carbon dioxide(CO_(2))batteries hold great promise for reducing greenhouse gas emissions and are regarded as one of the most promising energy storage techniques due to their efficiency advantages in CO_(2)recovery and conversion.Moreover,rechargeable nonaqueous metal-CO_(2)batteries have attracted much attention due to their high theoretical energy density.However,the stability issues of the electrode-electrolyte interfaces of nonaqueous metal-CO_(2)(lithium(Li)/sodium(Na)/potassium(K)-CO_(2))batteries have been troubling its development,and a large number of related research in the field of electrolytes have conducted in recent years.This review retraces the short but rapid research history of nonaqueous metal-CO_(2)batteries with a detailed electrochemical mechanism analysis.Then it focuses on the basic characteristics and design principles of electrolytes,summarizes the latest achievements of various types of electrolytes in a timely manner and deeply analyzes the construction strategies of stable electrode-electrolyte interfaces for metal-CO_(2)batteries.Finally,the key issues related to electrolytes and interface engineering are fully discussed and several potential directions for future research are proposed.This review enriches a comprehensive understanding of electrolytes and interface engineering toward the practical applications of next-generation metal-CO_(2)batteries.展开更多
Organic-inorganic hybrid perovskite solar cells achieve remarkable efficiencies(>26%)yet face stability challenges.Quasi-2D alternating-cation-interlayer perovskites offer enhanced stability through hydrophobic spa...Organic-inorganic hybrid perovskite solar cells achieve remarkable efficiencies(>26%)yet face stability challenges.Quasi-2D alternating-cation-interlayer perovskites offer enhanced stability through hydrophobic spacer cations but suffer from vertical phase segregation and buried interface defects.Herein,we introduce dicyanodiamide(DCD)to simultaneously address these dual limitations in GA(MA)_(n)Pb_(n)I_(3n+1)perovskites.The guanidine group in DCD passivates undercoordinated Pb^(2+)and MA^(+)vacancies at the perovskite/TiO_(2)interface,while cyano groups eliminate oxygen vacancies in TiO_(2)via Ti^(4+)-CN coordination,reducing interfacial trap density by 73%with respect to the control sample.In addition,DCD regulates crystallization kinetics,suppressing low-n-phase aggregation and promoting vertical alignment of high-n phases,which benefit for carrier transport.This dual-functional modification enhances charge transport and stabilizes energy-level alignment.The optimized devices achieve a record power conversion efficiency of 21.54%(vs.19.05%control)and retain 94%initial efficiency after 1200 h,outperforming unmodified counterparts(84%retention).Combining defect passivation with phase homogenization,this work establishes a molecular bridge strategy to decouple stability-efficiency trade-offs in low-dimensional perovskites,providing a universal framework for interface engineering in high-performance optoelectronics.展开更多
CO_(2) hydrogenation to CH3OH is of great significance for achieving carbon neutrality.Here,we show a urea-assisted grinding strategy for synthesizing Cu-Zn-Ce ternary catalysts(CZC-G)with optimized interfacial synerg...CO_(2) hydrogenation to CH3OH is of great significance for achieving carbon neutrality.Here,we show a urea-assisted grinding strategy for synthesizing Cu-Zn-Ce ternary catalysts(CZC-G)with optimized interfacial synergy,achieving superior performance in CO_(2) hydrogenation to methanol.The CZC-G catalyst demonstrated exceptional methanol selectivity(96.8%)and a space-time yield of 73.6 gMeOH·kgcat^(–1)·h^(–1) under optimized conditions.Long-term stability tests confirmed no obvious deactivation over 100 h of continuous operation.Structural and mechanistic analyses revealed that the urea-assisted grinding method promotes the formation of Cu/Zn-O_(v)-Ce ternary interfaces and inhibits the reduction of ZnO,enabling synergistic interactions for efficient CO_(2) activation and selective stabilization of formate intermediates(HCOO^(*)),which are critical for methanol synthesis.In-situ diffuse reflectance infrared Fourier transform spectra and X-ray absorption spectroscopy studies elucidated the reaction pathway dominated by the formate mechanism,while suppressing the reverse water-gas shift reaction.This work underscores the critical role of synthetic methodologies in engineering interfacial structures,offering a strategy for designing high-performance catalysts for sustainable CO_(2) resource utilization.展开更多
The 2D/3D heterojunction perovskites have garnered increasing attention due to their exceptional moisture and thermal stability.However,few works have paid attention to the influence of the subsequent change process o...The 2D/3D heterojunction perovskites have garnered increasing attention due to their exceptional moisture and thermal stability.However,few works have paid attention to the influence of the subsequent change process of 2D/3D heterojunction PSC on the stability of PSCs.Moreover,the evolution of the interface and carrier dynamic behavior of the 2D/3D perovskite films with long-term operation has not been systematically developed befo re.In this work,the effects of 2D/3 D heterojunction evolution on the interface of perovskite films and different carrier dynamics during 2D/3D evolution are systematically analyzed for the first time.The decomposition of 2D/3D heterojunction in the perovskite film will have a certain impact on the surface and carrier dynamics behavior of perovskite.During the evolution of 2D/3D heterojunction,PbI_(2)crystals will appear,which will improve the interfacial energy level matching between the electron transport layer and perovskite film.With a long evolution time,some holes will appear on the surface of perovskite film.The open circuit voltage(V_(OC))of PSCs increased from 1.14 to1.18 V and the PCE increased to 23.21%after 300 h storage in the nitrogen atmosphere,and maintained 89%initial performance for with 3000 h stability test in N_(2)box.This discovery has a significant role in promoting the development of inverted heterojunction PSCs and constructing the revolution mechanism of charge carrier dynamic.展开更多
Transition metal-carbonate interfaces often act as active sites in heterogeneous catalytic reactions.The interface between transition metal and metal carbonate exhibits a dynamic equilibrium during the CO_(2)hydrogena...Transition metal-carbonate interfaces often act as active sites in heterogeneous catalytic reactions.The interface between transition metal and metal carbonate exhibits a dynamic equilibrium during the CO_(2)hydrogenation reaction,involving surface carbonate hydrogenation and CO_(2)chemisorption.Nonetheless,there have been few reports on engineering the activity of the interface between transition metal and alkaline earth metal carbonate for catalytic CO_(2)conversion.This work demonstrated that the incorporation of CaH_(2)in Ni/CaCO_(3)enhances the CO_(2)methanation activity of the catalysts.The CO_(2)conversion for Ni/CaH_(2)-CaCO_(3)reached 68.5%at 400°C,which was much higher than that of the Ni/CaCO_(3)(31.6%) and Ni/CaH_(2)-CaO (42.4%) catalysts.Furthermore,the Ni/CaH_(2)-CaCO_(3)catalysts remained stable during the stability test for 24 h at 400°C and 8 bar.Our research revealed that CaH_(2)played a crucial role in promoting the activity of the Ni-carbonate interface for CO_(2)methanation.CaH_(2)could modify the electronic structure of Ni and tune the structural properties of CaCO_(3)to generate medium basic sites (OH groups),which are favorable for the activation of H2and CO_(2).In-situ Fourier transform infrared spectroscopy (FTIR) analysis combined with density functional theory calculations demonstrated that CO_(2)activation occurs at the hydroxyl group (OH) on the CaH_(2)-modified Ni-carbonate surface,leading to the formation of CO_(3)H*species.Furthermore,our study has confirmed that CO_(2)methanation over the Ni/CaH_(2)-CaCO_(3)catalysts proceeds via the formate pathway.展开更多
Efficient photocatalytic water splitting can be significantly enhanced through the careful design of S-scheme heterostructures,which play a pivotal role in optimizing performance.Herein,we report the construction of Z...Efficient photocatalytic water splitting can be significantly enhanced through the careful design of S-scheme heterostructures,which play a pivotal role in optimizing performance.Herein,we report the construction of ZnIn_(2)S_(4)/CdS S-scheme heterojunctions under ambient conditions,based on a sonochemical strategy.This structure is facilitated by the well-matched interface between the(007)plane of layered ZnIn_(2)S_(4)and the(101)plane of CdS,leading to a threshold optical response of 2.12 eV,which optimally aligns with visible light absorption.As a proof of concept,the resulting ZnIn_(2)S_(4)/CdS catalysts demonstrate a remarkable improvement in photocatalytic H_(2) evolution,achieving a rate of 5678.2μmol h^(-1)g^(-1)under visible light irradiation(λ>400 nm).This rate is approximately 10 times higher than that of pristine ZnIn_(2)S_(4)nanosheets(NSs)and about 4.6 times higher than that of CdS nanoparticles(NPs),surpassing the performance of most ZnIn_(2)S_(4)-based photocatalysts reported to date.Moreover,they deliver a robust photocatalytic performance during long-term operation of up to 60 h,showing their potential for use in practical applications.Based on the theoretical calculation and experimental results,it is verified that the movements of electrons and holes in the opposite direction could be induced by the disparity in the work function and the internal electric field within the interfaces,thus facilitating the construction of S-scheme heterojunctions,which fundamentally suppresses carrier recombination while minimizing photocorrosion of ZnIn_(2)S_(4)toward enhanced photocatalytic behaviors.展开更多
The development of dual functional material for cyclic CO_(2)capture and hydrogenation is of great significance for converting diluted CO_(2)into valuable fuels,but suffers from kinetic limitation and deactivation of ...The development of dual functional material for cyclic CO_(2)capture and hydrogenation is of great significance for converting diluted CO_(2)into valuable fuels,but suffers from kinetic limitation and deactivation of adsorbent and catalyst.Herein,we engineered a series of RuNa/γ-Al_(2)O_(3)materials,varying the size of ruthenium from single atoms to clusters/nanoparticles.The coordination environment and structure sensitivity of ruthenium were quantitatively investigated at atomic scale.Our findings reveal that the reduced Ru nanoparticles,approximately 7.1 nm in diameter with a Ru-Ru coordination number of 5.9,exhibit high methane formation activity and selectivity at 340°C.The Ru-Na interfacial sites facilitate CO_(2)migration through a deoxygenation pathway,involving carbonate dissociation,carbonyl formation,and hydrogenation.In-situ experiments and theoretical calculations show that stable carbonyl intermediates on metallic Ru nanoparticles facilitate heterolytic C–O scission and C–H bonding,significantly lowering the energy barrier for activating stored CO_(2).展开更多
The photocatalytic reduction of CO_(2)presents a promising avenue for carbon fuel conversion.However,the efficiency of charge utilization remains a critical barrier to industrial applications.In this study,we introduc...The photocatalytic reduction of CO_(2)presents a promising avenue for carbon fuel conversion.However,the efficiency of charge utilization remains a critical barrier to industrial applications.In this study,we introduce a tandem design of Bi_(2)WO_(6)-BiOCl with an atomically matched interface,achieving highly efficient photoreduction of CO_(2)to CO.By incorporating WO_(4)^(2-)ions and tuning coordination environment,the(110)facet of BiOCl was in-situ grown on the(200)facet of Bi_(2)WO_(6).Compared to single phases and ball-milling samples,Bi_(2)WO_(6)-BiOCl exhibits a remarkable CO yield of 68.03μmol g^(-1)h^(-1)with a selectivity of 98%.Atomic visualization and coordination analysis confirm the formation of a coherent interface that facilitates charge migration for efficient electron transport.Density functional theory(DFT)calculations and in-situ Fourier transform infrared(FTIR)spectroscopy provide insights into the intrinsic active sites and reaction mechanisms.The proposed lattice engineering strategies offer a new paradigm for the rational design of heterostructures beyond traditional band alignment at the atomic scale.展开更多
The interface modulation significantly affects the photocatalytic performances of supported metal phthalocyanines(MPc)-based systems.Herein,ZnPc was loaded on nanosized Au-modified TiO_(2)nanosheets(Au-T)to obtain wid...The interface modulation significantly affects the photocatalytic performances of supported metal phthalocyanines(MPc)-based systems.Herein,ZnPc was loaded on nanosized Au-modified TiO_(2)nanosheets(Au-T)to obtain wide-spectrum ZnPc/Au-T photocatalysts.Compared with large Au NP(8 nm)-mediated ZnPc/Au-T photocatalyst,ultrasmall Au NP(3 nm)-mediated one shows advantageous photoactivity,achieving 3-and 10-fold CO_(2)conversion rates compared with reference ZnPc/T and pristine TiO_(2)nanosheets,respectively.Employing monochromatic beam-assisted surface photovoltage and photocurrent action,etc.,the introduction of ultrasmall Au NPs more effectively facilitates intrinsic interfacial charge transfer.Moreover,ZnP c molecules are found more dispersed with the existence of small Au NPs hence exposing abundant Zn^(2+)sites as the catalytic center for CO_(2)reduction.This work provides a feasible design strategy and renewed recognition for supported MPc-based photocatalyst systems.展开更多
Lithium-carbon dioxide(Li-CO_(2))batteries with high theoretical energy density are regarded as promising energy storage system toward carbon neutrality.However,bidirectional catalysts design for improving the sluggis...Lithium-carbon dioxide(Li-CO_(2))batteries with high theoretical energy density are regarded as promising energy storage system toward carbon neutrality.However,bidirectional catalysts design for improving the sluggish CO_(2)reduction reaction(CO_(2)RR)/CO_(2)evolution reaction(CO_(2)ER)kinetics remains a huge challenge.In this work,an advanced catalyst with fast-interfacial charge transfer was subtly synthesized through element segregation,which significantly improves the electrocatalytic activity for both CO_(2)RR and CO_(2)ER.Theoretical calculations and characterization analysis demonstrate local charge redistribution at the constructed interface,which leads to optimized binding affinity towards reactants and preferred Li_(2)CO_(3)decomposition behavior,enabling excellent catalytic activity during CO_(2)redox.Benefiting from the enhanced charge transfer ability,the designed highly efficient catalyst with dual active centers and large exposed catalytic area can maintain an ultra-small voltage gap of 0.33 V and high energy efficiency of 90.2%.This work provides an attractive strategy to construct robust catalysts by interface engineering,which could inspire further design of superior bidirectional catalysts for Li-CO_(2)batteries.展开更多
Modulating the interface between the electron transport layer(ETL)and perovskite to minimize interfacial recombination is pivotal for developing efficient and stable perovskite solar cells.Here,we introduce an ultra-t...Modulating the interface between the electron transport layer(ETL)and perovskite to minimize interfacial recombination is pivotal for developing efficient and stable perovskite solar cells.Here,we introduce an ultra-thin ZrO_(2)insulating interface layer onto the inner surface of the mesoporous TiO_(2)ETL via the chemical bath deposition in the zirconium n-butoxide solution,which alters the interface characteristics between TiO_(2)and perovskite for the printable hole-conductor-free mesoscopic perovskite solar cells(p-MPSCs).The insulating ZrO_(2)interface layer reduces interface defects and suppresses interfacial non-radiative recombination.Furthermore,the ZrO_(2)interface layer improves the wettability of the mesoporous TiO_(2)ETL,which favors the crystallization of perovskite within the mesoporous scaffold.Meanwhile,the device performance presents thickness dependence on the interface layer.While increased thickness improves the open-circuit voltage,excessive thickness negatively impacts both the short-circuit current density and fill factor.Consequently,an improved power conversion efficiency of 19.9% was achieved for p-MPSCs with the ZrO_(2)interface layer at its optimized thickness.展开更多
Sodium-ion batteries with ZnIn_(2)S_(4)(ZIS)anodes promise a high capacity and abundant resources.However,their inherent low conductivity,large volume expansion and sluggish Na+diffusion limit the development of the w...Sodium-ion batteries with ZnIn_(2)S_(4)(ZIS)anodes promise a high capacity and abundant resources.However,their inherent low conductivity,large volume expansion and sluggish Na+diffusion limit the development of the wide-temperature sodium storage.This study pioneers a scalable synthesis of hierarchical hollow structural ZIS/C heterostructure through in situ confined growth of ZIS nanosheets in porous hollow carbon spheres(PHCSs)via a hydrothermal method.This unique structure exhibits abundant heterostructures to facilitate charge transport,rich porous structures to promote electrolyte wettability,efficient space utilization to relieve volume expansion,as well as interconnected carbon networks to ensure framework stability.Consequently,ZIS/C exhibits exceptional cycling stability with 92%capacity retention after 1000 cycles.Notably,ZIS/C demonstrates good wide-temperature performance operating at–50∼90°C,especially,at–30°C with a capacity of 208 mA h g^(−1)at 0.3A g^(−1).The full cell of ZIS/C||Na_(3)V_(2)(PO_(4))_(3)exhibits excellent high-rate capability(178 mA h g^(−1)at 6A g^(−1)).展开更多
Metal-ceramic composites combine the excellent properties of metals and ceramics,which have high strength,stability,and corrosion re-sistance.Al_(2)O_(3)/FeCo composites have been proven to be useful in ap-plications ...Metal-ceramic composites combine the excellent properties of metals and ceramics,which have high strength,stability,and corrosion re-sistance.Al_(2)O_(3)/FeCo composites have been proven to be useful in ap-plications such as catalysts,mi-crowave absorption materials,and enhanced permeability dielectric.The understanding of the mechani-cal properties and dynamics at the atomic scale of the Al_(2)O_(3)/FeCo in-terface can promote the design and exploitment of metal-ceramic composites.In this work,we have obtained Young’s modulus and diffusion coefficient of the Al_(2)O_(3)/FeCo interface using molecular dynamics simulation,elucidated the structural characteristics of the Al_(2)O_(3)/FeCo interface at the atomic scale,and investigated the impact of atomic magnetism and the exter-nal magnetic field on the interface.Simulated results show that Young’s modulus of the Al_(2)O_(3)/FeCo interface is significantly improved compared with pure Al_(2)O_(3)and FeCo alloy at room and high temperatures.When the atomic magnetism and the external magnetic field are applied,Young’s modulus of the Al_(2)O_(3)/FeCo interface further increases to 612 GPa at 300 K and 602 GPa at 500 K.Moreover,the average density,diffusion coefficient,and radial distri-bution function are found to be modified substantially.This study will shed light on the atom-istic investigations of the metal-ceramic composites.展开更多
Water transport at the root/soil interface of 1 year old Pinus sylvestris Linn. var. sylvestriformis (Takenouchi) Cheng et C. D. Chu seedlings under CO 2 doubling was studied by measuring soil electric conductanc...Water transport at the root/soil interface of 1 year old Pinus sylvestris Linn. var. sylvestriformis (Takenouchi) Cheng et C. D. Chu seedlings under CO 2 doubling was studied by measuring soil electric conductance to survey soil water profiles and comparing it with root distribution surveyed by soil coring and root harvesting in Changbai Mountain in 1999. The results were: (1) The profiles of soil water content were adjusted by root activity. The water content of the soil layer with abundant roots was higher. (2) When CO 2 concentration was doubled, water transport was more active at the root/soil interface and the roots were distributed into deeper layer. It was shown in this work that the method of measuring electric conductance is an inexpensive, non_destructive and relatively sensitive way for underground water transport process.展开更多
Electrocatalytic CO_(2) reduction reaction(CO_(2) RR) can store and transform the intermittent renewable energy in the form of chemical energy for industrial production of chemicals and fuels,which can dramatically re...Electrocatalytic CO_(2) reduction reaction(CO_(2) RR) can store and transform the intermittent renewable energy in the form of chemical energy for industrial production of chemicals and fuels,which can dramatically reduce CO_(2) emission and contribute to carbon-neutral cycle. E cient electrocatalytic reduction of chemically inert CO_(2) is challenging from thermodynamic and kinetic points of view. Therefore,low-cost,highly e cient,and readily available electrocatalysts have been the focus for promoting the conversion of CO_(2). Very recently,interface engineering has been considered as a highly e ective strategy to modulate the electrocatalytic performance through electronic and/or structural modulation,regulations of electron/proton/mass/intermediates,and the control of local reactant concentration,thereby achieving desirable reaction pathway,inhibiting competing hydrogen generation,breaking binding-energy scaling relations of intermediates,and promoting CO_(2) mass transfer. In this review,we aim to provide a comprehensive overview of current developments in interface engineering for CO_(2) RR from both a theoretical and experimental stand-point,involving interfaces between metal and metal,metal and metal oxide,metal and nonmetal,metal oxide and metal oxide,organic molecules and inorganic materials,electrode and electrolyte,molecular catalysts and electrode,etc. Finally,the opportunities and challenges of interface engineering for CO_(2) RR are proposed.展开更多
High ionic conductivity and superior interfacial stability of solid electrolytes at the electrodes are crucial factors for high-performance all-solid-state sodium batteries. Herein, a composite solid electrolyte Na3PS...High ionic conductivity and superior interfacial stability of solid electrolytes at the electrodes are crucial factors for high-performance all-solid-state sodium batteries. Herein, a composite solid electrolyte Na3PS4-polyethylene oxide is synthesized by the solution-phase reaction method with an improved ionic conductivity up to 9.4 × 10-5 S/cm at room temperature. Moreover, polyethylene oxide polymer layer is wrapped homogeneously on the surface of Na3PS4 particles, which could effectively avoid the direct contact between Na3PS4 electrolyte and sodium metal, thus alleviate their side reactions. We demonstrate that all-solid-state battery SnS2/Na with the composite solid electrolyte Na3PS4-polyethylene oxide delivers an enhanced electrochemical performance with 230 m Ah/g after 40 cycles.展开更多
Tin dioxide(SnO_(2))has been demonstrated as one of the promising electron transport layers for high-efficiency perovskite solar cells(PSCs).However,scalable fabrication of SnO_(2) films with uniform coverage,desirabl...Tin dioxide(SnO_(2))has been demonstrated as one of the promising electron transport layers for high-efficiency perovskite solar cells(PSCs).However,scalable fabrication of SnO_(2) films with uniform coverage,desirable thickness and a low defect density in perovskite solar mod-ules(PSMs)is still challenging.Here,we report preparation of high-quality large-area SnO_(2) films by chemical bath depo-sition(CBD)with the addition of KMnO_(4).The strong oxidiz-ing nature of KMnO_(4) promotes the conversion from Sn(II)to Sn(VI),leading to reduced trap defects and a higher carrier mobility of SnO_(2).In addition,K ions diffuse into the per-ovskite film resulting in larger grain sizes,passivated grain boundaries,and reduced hysteresis of PSCs.Furthermore,Mn ion doping improves both the crystallinity and the phase stability of the perovskite film.Such a multifunctional interface engineering strategy enabled us to achieve a power conversion efficiency(PCE)of 21.70% with less hysteresis for lab-scale PSCs.Using this method,we also fabricated 5×5 and 10×10 cm^(2) PSMs,which showed PCEs of 15.62% and 11.80%(active area PCEs are 17.26%and 13.72%),respectively.For the encapsulated 5×5 cm^(2) PSM,we obtained a T80 operation lifetime(the lifespan during which the solar module PCE drops to 80%of its initial value)exceeding 1000 h in ambient condition.展开更多
The electrochemical CO_(2)reduction reaction to produce multi-carbon(C_(2+)) hydrocarbons or oxygenate compounds is a promising route to obtain a renewable fuel of high energy density.However,producing C_(2+)at high c...The electrochemical CO_(2)reduction reaction to produce multi-carbon(C_(2+)) hydrocarbons or oxygenate compounds is a promising route to obtain a renewable fuel of high energy density.However,producing C_(2+)at high current densities is still a challenge.Herein,we develop a Cu-Zn alloy/Cu-Zn aluminate oxide composite electrocatalytic system for enhanced conversion of CO_(2)to C_(2+)products.The Cu-Zn-Al-Layered Double Hydroxide(LDH) is used as a precursor to decompose into uniform Cu-Zn oxide/Cu-Zn aluminate pre-catalyst.Under electrochemical reduction,Cu-Zn oxide generates Cu-Zn alloy while Cu-Zn aluminate oxide remains unchanged.The alloy and oxide are closely stacked and arranged alternately,and the aluminate oxide induces the strong electron interaction of Cu,Zn and Al,creating a large number of highly active reaction interfaces composed of 0 to+3 valence metal sites.With the help of the interface effect,the optimized Cu_(9)Zn_(1)/Cu_(0.8)Zn_(0.2)Al_(2)O_(4)catalyst achieves a Faradaic efficiency of 88.5% for C_(2+)products at a current density of 400 mA cm^(-2)at-1.15 V versus reversible hydrogen electrode.The in-situ Raman and attenuate total reflectance-infrared absorption spectroscopy(ATR-IRAS) spectra show that the aluminate oxide at the interface significantly enhances the adsorption and activation of CO_(2)and the dissociation of H2O and strengthens the adsorption of CO intermediates,and the alloy promotes the C-C coupling to produce C_(2+)products.This work provides an efficient strategy to construct highly active reaction interfaces for industrial-scale electrochemical CO_(2)RR.展开更多
文摘A CuPc/SiO2 sample is fabricated. Its morphology is characterized by atomic force microscopy, and the electron states are investigated by X-ray photoelectron spectroscopy. In order to investigate these spectra in detail, all of these spectra are normalized to the height of the most intense peak,and each component is fitted with a single Gaussian function. Analysis shows that the O element has great bearing on the electron states and that SiO2 layers produced by spurting technology are better than those produced by oxidation technology.
文摘CeO_(2) based semiconductor are widely used in solar-driven photothermal catalytic dry reforming of methane(DRM)reaction,but still suffer from low activity and low light utilization efficiency.This study developed graphite-CeO_(2) interfaces to enhance solar-driven photothermal catalytic DRM.Compared with carbon nanotubes-modified CeO_(2)(CeO_(2)-CNT),graphite-modified CeO_(2)(CeO_(2)-GRA)constructed graphite-CeO_(2) interfaces with distortion in CeO_(2),leading to the formation abundant oxygen vacancies.These graphite-CeO_(2) interfaces with oxygen vacancies enhanced optical absorption and promoted the generation and separation of photogenerated carriers.The high endothermic capacity of graphite elevated the catalyst surface temperature from 592.1−691.3℃,boosting light-to-thermal conversion.The synergy between photogenerated carriers and localized heat enabled Ni/CeO_(2)-GRA to achieve a CO production rate of 9985.6 mmol/(g·h)(vs 7192.4 mmol/(g·h)for Ni/CeO_(2))and a light-to-fuel efficiency of 21.8%(vs 13.8%for Ni/CeO_(2)).This work provides insights for designing graphite-semiconductor interfaces to advance photothermal catalytic efficiency.
基金supports from the Beijing Laboratory of New Energy Storage Technology, North China Electric Power Universitythe Program of the National Energy Storage Industry-Education Platformthe Interdisciplinary Innovation Program of North China Electric Power University (No. XM2212315)
文摘Metal-carbon dioxide(CO_(2))batteries hold great promise for reducing greenhouse gas emissions and are regarded as one of the most promising energy storage techniques due to their efficiency advantages in CO_(2)recovery and conversion.Moreover,rechargeable nonaqueous metal-CO_(2)batteries have attracted much attention due to their high theoretical energy density.However,the stability issues of the electrode-electrolyte interfaces of nonaqueous metal-CO_(2)(lithium(Li)/sodium(Na)/potassium(K)-CO_(2))batteries have been troubling its development,and a large number of related research in the field of electrolytes have conducted in recent years.This review retraces the short but rapid research history of nonaqueous metal-CO_(2)batteries with a detailed electrochemical mechanism analysis.Then it focuses on the basic characteristics and design principles of electrolytes,summarizes the latest achievements of various types of electrolytes in a timely manner and deeply analyzes the construction strategies of stable electrode-electrolyte interfaces for metal-CO_(2)batteries.Finally,the key issues related to electrolytes and interface engineering are fully discussed and several potential directions for future research are proposed.This review enriches a comprehensive understanding of electrolytes and interface engineering toward the practical applications of next-generation metal-CO_(2)batteries.
基金support from the National Key R&D Program of China(Grant No.2023YFE0111500)the National Natural Science Foundation of China(Grant No.52321006,T2394480,T2394484,22109143,22479131)+8 种基金Beijing National Laboratory for Molecular Sciences(BNLMS-CXXM-202005)the China Postdoctoral Innovative Talent Support Program(Grant No.BX2021271)the China Postdoctoral Science Foundation(2022M712851)the Opening Project of State Key Laboratory of Advanced Technology for Float Glass(Grant No.2022KF04)Graduate Education Reform Project of Henan Province(Grant No.2023SJGLX136Y)Key R&D Special Program of Henan Province(Grant No.241111242000)Program for Science and Technology Innovation Talents in Universities of Henan Province(Grant No.25HASTIT005)Training Plan for Young Backbone Teachers of Zhengzhou University(Grant No.2023ZDGGJS017)the Joint Research Project of Puyang Shengtong Juyuan New Materials Co.,Ltd.(Grant No.20230128A).
文摘Organic-inorganic hybrid perovskite solar cells achieve remarkable efficiencies(>26%)yet face stability challenges.Quasi-2D alternating-cation-interlayer perovskites offer enhanced stability through hydrophobic spacer cations but suffer from vertical phase segregation and buried interface defects.Herein,we introduce dicyanodiamide(DCD)to simultaneously address these dual limitations in GA(MA)_(n)Pb_(n)I_(3n+1)perovskites.The guanidine group in DCD passivates undercoordinated Pb^(2+)and MA^(+)vacancies at the perovskite/TiO_(2)interface,while cyano groups eliminate oxygen vacancies in TiO_(2)via Ti^(4+)-CN coordination,reducing interfacial trap density by 73%with respect to the control sample.In addition,DCD regulates crystallization kinetics,suppressing low-n-phase aggregation and promoting vertical alignment of high-n phases,which benefit for carrier transport.This dual-functional modification enhances charge transport and stabilizes energy-level alignment.The optimized devices achieve a record power conversion efficiency of 21.54%(vs.19.05%control)and retain 94%initial efficiency after 1200 h,outperforming unmodified counterparts(84%retention).Combining defect passivation with phase homogenization,this work establishes a molecular bridge strategy to decouple stability-efficiency trade-offs in low-dimensional perovskites,providing a universal framework for interface engineering in high-performance optoelectronics.
文摘CO_(2) hydrogenation to CH3OH is of great significance for achieving carbon neutrality.Here,we show a urea-assisted grinding strategy for synthesizing Cu-Zn-Ce ternary catalysts(CZC-G)with optimized interfacial synergy,achieving superior performance in CO_(2) hydrogenation to methanol.The CZC-G catalyst demonstrated exceptional methanol selectivity(96.8%)and a space-time yield of 73.6 gMeOH·kgcat^(–1)·h^(–1) under optimized conditions.Long-term stability tests confirmed no obvious deactivation over 100 h of continuous operation.Structural and mechanistic analyses revealed that the urea-assisted grinding method promotes the formation of Cu/Zn-O_(v)-Ce ternary interfaces and inhibits the reduction of ZnO,enabling synergistic interactions for efficient CO_(2) activation and selective stabilization of formate intermediates(HCOO^(*)),which are critical for methanol synthesis.In-situ diffuse reflectance infrared Fourier transform spectra and X-ray absorption spectroscopy studies elucidated the reaction pathway dominated by the formate mechanism,while suppressing the reverse water-gas shift reaction.This work underscores the critical role of synthetic methodologies in engineering interfacial structures,offering a strategy for designing high-performance catalysts for sustainable CO_(2) resource utilization.
基金financial support provided by the Sichuan Science and Technology Program(No.2022NSFSC0226)Sichuan Science and Technology Program(No.2023ZYD0163)+6 种基金the Production-Education Integration Demonstration Project of Sichuan Provincethe Photovoltaic Industry Production-Education Integration Comprehensive Demonstration Base of Sichuan Province(Sichuan Financial Education[2022]No.106)China Tianfu Yongxing Laboratory Science and Technology Key Project(2023KJGG15)National Key Research and Development Program of China(2022YFB3803300)Beijing Natural Science Foundation(IS23037)the Department for Energy Security and Net Zero(project ID:NEXTCCUS)the ACT program(Accelerating CCS Technologies,Horizon2020 project NO.691712)。
文摘The 2D/3D heterojunction perovskites have garnered increasing attention due to their exceptional moisture and thermal stability.However,few works have paid attention to the influence of the subsequent change process of 2D/3D heterojunction PSC on the stability of PSCs.Moreover,the evolution of the interface and carrier dynamic behavior of the 2D/3D perovskite films with long-term operation has not been systematically developed befo re.In this work,the effects of 2D/3 D heterojunction evolution on the interface of perovskite films and different carrier dynamics during 2D/3D evolution are systematically analyzed for the first time.The decomposition of 2D/3D heterojunction in the perovskite film will have a certain impact on the surface and carrier dynamics behavior of perovskite.During the evolution of 2D/3D heterojunction,PbI_(2)crystals will appear,which will improve the interfacial energy level matching between the electron transport layer and perovskite film.With a long evolution time,some holes will appear on the surface of perovskite film.The open circuit voltage(V_(OC))of PSCs increased from 1.14 to1.18 V and the PCE increased to 23.21%after 300 h storage in the nitrogen atmosphere,and maintained 89%initial performance for with 3000 h stability test in N_(2)box.This discovery has a significant role in promoting the development of inverted heterojunction PSCs and constructing the revolution mechanism of charge carrier dynamic.
基金National Natural Science Foundation of China (Nos. 22371244 and 21573192)Postgraduate Research&Practice Innovation Program of Jiangsu Province(KYCX22_3463)。
文摘Transition metal-carbonate interfaces often act as active sites in heterogeneous catalytic reactions.The interface between transition metal and metal carbonate exhibits a dynamic equilibrium during the CO_(2)hydrogenation reaction,involving surface carbonate hydrogenation and CO_(2)chemisorption.Nonetheless,there have been few reports on engineering the activity of the interface between transition metal and alkaline earth metal carbonate for catalytic CO_(2)conversion.This work demonstrated that the incorporation of CaH_(2)in Ni/CaCO_(3)enhances the CO_(2)methanation activity of the catalysts.The CO_(2)conversion for Ni/CaH_(2)-CaCO_(3)reached 68.5%at 400°C,which was much higher than that of the Ni/CaCO_(3)(31.6%) and Ni/CaH_(2)-CaO (42.4%) catalysts.Furthermore,the Ni/CaH_(2)-CaCO_(3)catalysts remained stable during the stability test for 24 h at 400°C and 8 bar.Our research revealed that CaH_(2)played a crucial role in promoting the activity of the Ni-carbonate interface for CO_(2)methanation.CaH_(2)could modify the electronic structure of Ni and tune the structural properties of CaCO_(3)to generate medium basic sites (OH groups),which are favorable for the activation of H2and CO_(2).In-situ Fourier transform infrared spectroscopy (FTIR) analysis combined with density functional theory calculations demonstrated that CO_(2)activation occurs at the hydroxyl group (OH) on the CaH_(2)-modified Ni-carbonate surface,leading to the formation of CO_(3)H*species.Furthermore,our study has confirmed that CO_(2)methanation over the Ni/CaH_(2)-CaCO_(3)catalysts proceeds via the formate pathway.
基金supported by the National Natural Science Foundation of China(NSFC,Grant No.52372063,62204246 and 52401244)the Young Elite Scientists Sponsorship Program by CAST(Grant No.2023QNRC001)+1 种基金the Postdoctoral Fellowship Program of CPSF(Grant No.GZC20233001,GZC20233006)the China Postdoctoral Science Foundation(Grant No.2024M753526)。
文摘Efficient photocatalytic water splitting can be significantly enhanced through the careful design of S-scheme heterostructures,which play a pivotal role in optimizing performance.Herein,we report the construction of ZnIn_(2)S_(4)/CdS S-scheme heterojunctions under ambient conditions,based on a sonochemical strategy.This structure is facilitated by the well-matched interface between the(007)plane of layered ZnIn_(2)S_(4)and the(101)plane of CdS,leading to a threshold optical response of 2.12 eV,which optimally aligns with visible light absorption.As a proof of concept,the resulting ZnIn_(2)S_(4)/CdS catalysts demonstrate a remarkable improvement in photocatalytic H_(2) evolution,achieving a rate of 5678.2μmol h^(-1)g^(-1)under visible light irradiation(λ>400 nm).This rate is approximately 10 times higher than that of pristine ZnIn_(2)S_(4)nanosheets(NSs)and about 4.6 times higher than that of CdS nanoparticles(NPs),surpassing the performance of most ZnIn_(2)S_(4)-based photocatalysts reported to date.Moreover,they deliver a robust photocatalytic performance during long-term operation of up to 60 h,showing their potential for use in practical applications.Based on the theoretical calculation and experimental results,it is verified that the movements of electrons and holes in the opposite direction could be induced by the disparity in the work function and the internal electric field within the interfaces,thus facilitating the construction of S-scheme heterojunctions,which fundamentally suppresses carrier recombination while minimizing photocorrosion of ZnIn_(2)S_(4)toward enhanced photocatalytic behaviors.
基金National Key R&D Program of China(2022YFE0105900)National Natural Science Foundation of China(52306179)+1 种基金Science and Technology Innovation Program of Hunan Province(2021RC4006)High Performance Computing Center of Central South University。
文摘The development of dual functional material for cyclic CO_(2)capture and hydrogenation is of great significance for converting diluted CO_(2)into valuable fuels,but suffers from kinetic limitation and deactivation of adsorbent and catalyst.Herein,we engineered a series of RuNa/γ-Al_(2)O_(3)materials,varying the size of ruthenium from single atoms to clusters/nanoparticles.The coordination environment and structure sensitivity of ruthenium were quantitatively investigated at atomic scale.Our findings reveal that the reduced Ru nanoparticles,approximately 7.1 nm in diameter with a Ru-Ru coordination number of 5.9,exhibit high methane formation activity and selectivity at 340°C.The Ru-Na interfacial sites facilitate CO_(2)migration through a deoxygenation pathway,involving carbonate dissociation,carbonyl formation,and hydrogenation.In-situ experiments and theoretical calculations show that stable carbonyl intermediates on metallic Ru nanoparticles facilitate heterolytic C–O scission and C–H bonding,significantly lowering the energy barrier for activating stored CO_(2).
基金supported by the National Key R&D Program of China(No.2021YFA1200201)the Beijing Outstanding Young Scientists Projects(No.BJJWZYJH01201910005018)+1 种基金The Basic Science Center Program for Multiphase Evolution in Hypergravity of the National Natural Science Foundation of China(No.51988101)the National Natural Science Foundation of China(Nos.52071003 and 91860202)。
文摘The photocatalytic reduction of CO_(2)presents a promising avenue for carbon fuel conversion.However,the efficiency of charge utilization remains a critical barrier to industrial applications.In this study,we introduce a tandem design of Bi_(2)WO_(6)-BiOCl with an atomically matched interface,achieving highly efficient photoreduction of CO_(2)to CO.By incorporating WO_(4)^(2-)ions and tuning coordination environment,the(110)facet of BiOCl was in-situ grown on the(200)facet of Bi_(2)WO_(6).Compared to single phases and ball-milling samples,Bi_(2)WO_(6)-BiOCl exhibits a remarkable CO yield of 68.03μmol g^(-1)h^(-1)with a selectivity of 98%.Atomic visualization and coordination analysis confirm the formation of a coherent interface that facilitates charge migration for efficient electron transport.Density functional theory(DFT)calculations and in-situ Fourier transform infrared(FTIR)spectroscopy provide insights into the intrinsic active sites and reaction mechanisms.The proposed lattice engineering strategies offer a new paradigm for the rational design of heterostructures beyond traditional band alignment at the atomic scale.
基金supported by the National Natural Science Foundation of China(Nos.U2102211 and 22378101)the Fundamental Research Foundation for Universities of Heilongjiang Province(No.2021-KYYWF-0004)the Science Fund for Distinguished Young Scholars of Heilongjiang University(No.JCL202102)。
文摘The interface modulation significantly affects the photocatalytic performances of supported metal phthalocyanines(MPc)-based systems.Herein,ZnPc was loaded on nanosized Au-modified TiO_(2)nanosheets(Au-T)to obtain wide-spectrum ZnPc/Au-T photocatalysts.Compared with large Au NP(8 nm)-mediated ZnPc/Au-T photocatalyst,ultrasmall Au NP(3 nm)-mediated one shows advantageous photoactivity,achieving 3-and 10-fold CO_(2)conversion rates compared with reference ZnPc/T and pristine TiO_(2)nanosheets,respectively.Employing monochromatic beam-assisted surface photovoltage and photocurrent action,etc.,the introduction of ultrasmall Au NPs more effectively facilitates intrinsic interfacial charge transfer.Moreover,ZnP c molecules are found more dispersed with the existence of small Au NPs hence exposing abundant Zn^(2+)sites as the catalytic center for CO_(2)reduction.This work provides a feasible design strategy and renewed recognition for supported MPc-based photocatalyst systems.
基金supported by the National Key Research and Development Program of China(2019YFA0705700)Guangdong Innovative and Entrepreneurial Research Team Program(2021ZT09L197)+2 种基金Shenzhen Science and Technology Program(KQTD20210811090112002)Interdisciplinary Research and Innovation Fund of Tsinghua Shenzhen International Graduate School,National Natural Science Foundation of China(No.52373233)the SIAT International Joint Lab Project(No.E3G113).
文摘Lithium-carbon dioxide(Li-CO_(2))batteries with high theoretical energy density are regarded as promising energy storage system toward carbon neutrality.However,bidirectional catalysts design for improving the sluggish CO_(2)reduction reaction(CO_(2)RR)/CO_(2)evolution reaction(CO_(2)ER)kinetics remains a huge challenge.In this work,an advanced catalyst with fast-interfacial charge transfer was subtly synthesized through element segregation,which significantly improves the electrocatalytic activity for both CO_(2)RR and CO_(2)ER.Theoretical calculations and characterization analysis demonstrate local charge redistribution at the constructed interface,which leads to optimized binding affinity towards reactants and preferred Li_(2)CO_(3)decomposition behavior,enabling excellent catalytic activity during CO_(2)redox.Benefiting from the enhanced charge transfer ability,the designed highly efficient catalyst with dual active centers and large exposed catalytic area can maintain an ultra-small voltage gap of 0.33 V and high energy efficiency of 90.2%.This work provides an attractive strategy to construct robust catalysts by interface engineering,which could inspire further design of superior bidirectional catalysts for Li-CO_(2)batteries.
基金financial support from the National Natural Science Foundation of China(22439001,52172198,51902117)supported by the Innovation Fund of Wuhan National Laboratory for Optoelectronicsthe Analytical and Testing Center of Huazhong University of Science and Technology(HUST)for performing various characterizations。
文摘Modulating the interface between the electron transport layer(ETL)and perovskite to minimize interfacial recombination is pivotal for developing efficient and stable perovskite solar cells.Here,we introduce an ultra-thin ZrO_(2)insulating interface layer onto the inner surface of the mesoporous TiO_(2)ETL via the chemical bath deposition in the zirconium n-butoxide solution,which alters the interface characteristics between TiO_(2)and perovskite for the printable hole-conductor-free mesoscopic perovskite solar cells(p-MPSCs).The insulating ZrO_(2)interface layer reduces interface defects and suppresses interfacial non-radiative recombination.Furthermore,the ZrO_(2)interface layer improves the wettability of the mesoporous TiO_(2)ETL,which favors the crystallization of perovskite within the mesoporous scaffold.Meanwhile,the device performance presents thickness dependence on the interface layer.While increased thickness improves the open-circuit voltage,excessive thickness negatively impacts both the short-circuit current density and fill factor.Consequently,an improved power conversion efficiency of 19.9% was achieved for p-MPSCs with the ZrO_(2)interface layer at its optimized thickness.
基金supported by the National Natural Science Foundation of China(U23B2075)the Natural Science Foundation of Shandong Province(ZR202111290333)the China Postdoctoral Science Foundation(2023M730640,2024M750490).
文摘Sodium-ion batteries with ZnIn_(2)S_(4)(ZIS)anodes promise a high capacity and abundant resources.However,their inherent low conductivity,large volume expansion and sluggish Na+diffusion limit the development of the wide-temperature sodium storage.This study pioneers a scalable synthesis of hierarchical hollow structural ZIS/C heterostructure through in situ confined growth of ZIS nanosheets in porous hollow carbon spheres(PHCSs)via a hydrothermal method.This unique structure exhibits abundant heterostructures to facilitate charge transport,rich porous structures to promote electrolyte wettability,efficient space utilization to relieve volume expansion,as well as interconnected carbon networks to ensure framework stability.Consequently,ZIS/C exhibits exceptional cycling stability with 92%capacity retention after 1000 cycles.Notably,ZIS/C demonstrates good wide-temperature performance operating at–50∼90°C,especially,at–30°C with a capacity of 208 mA h g^(−1)at 0.3A g^(−1).The full cell of ZIS/C||Na_(3)V_(2)(PO_(4))_(3)exhibits excellent high-rate capability(178 mA h g^(−1)at 6A g^(−1)).
基金supported by the National Natural Science Foundation of China(Nos.22173057,52130204,12074241,11929401,12311530675)Science and Technology Commission of Shanghai Municipality(Nos.21JC1402700,22XD1400900,20501130600,21JC1402600)High-Performance Computing Center,Shanghai Technical Service Center of Science and Engineering Computing,Shanghai University。
文摘Metal-ceramic composites combine the excellent properties of metals and ceramics,which have high strength,stability,and corrosion re-sistance.Al_(2)O_(3)/FeCo composites have been proven to be useful in ap-plications such as catalysts,mi-crowave absorption materials,and enhanced permeability dielectric.The understanding of the mechani-cal properties and dynamics at the atomic scale of the Al_(2)O_(3)/FeCo in-terface can promote the design and exploitment of metal-ceramic composites.In this work,we have obtained Young’s modulus and diffusion coefficient of the Al_(2)O_(3)/FeCo interface using molecular dynamics simulation,elucidated the structural characteristics of the Al_(2)O_(3)/FeCo interface at the atomic scale,and investigated the impact of atomic magnetism and the exter-nal magnetic field on the interface.Simulated results show that Young’s modulus of the Al_(2)O_(3)/FeCo interface is significantly improved compared with pure Al_(2)O_(3)and FeCo alloy at room and high temperatures.When the atomic magnetism and the external magnetic field are applied,Young’s modulus of the Al_(2)O_(3)/FeCo interface further increases to 612 GPa at 300 K and 602 GPa at 500 K.Moreover,the average density,diffusion coefficient,and radial distri-bution function are found to be modified substantially.This study will shed light on the atom-istic investigations of the metal-ceramic composites.
文摘Water transport at the root/soil interface of 1 year old Pinus sylvestris Linn. var. sylvestriformis (Takenouchi) Cheng et C. D. Chu seedlings under CO 2 doubling was studied by measuring soil electric conductance to survey soil water profiles and comparing it with root distribution surveyed by soil coring and root harvesting in Changbai Mountain in 1999. The results were: (1) The profiles of soil water content were adjusted by root activity. The water content of the soil layer with abundant roots was higher. (2) When CO 2 concentration was doubled, water transport was more active at the root/soil interface and the roots were distributed into deeper layer. It was shown in this work that the method of measuring electric conductance is an inexpensive, non_destructive and relatively sensitive way for underground water transport process.
基金supported by the National Natural Science Foundation of China (22071172)the Ministry of Science and Technology of China (2016YFB0401100,2017YFA0204503,and 2018YFA0703200)Shandong Provincial Natural Science Foundation (No. ZR2019BB025)。
文摘Electrocatalytic CO_(2) reduction reaction(CO_(2) RR) can store and transform the intermittent renewable energy in the form of chemical energy for industrial production of chemicals and fuels,which can dramatically reduce CO_(2) emission and contribute to carbon-neutral cycle. E cient electrocatalytic reduction of chemically inert CO_(2) is challenging from thermodynamic and kinetic points of view. Therefore,low-cost,highly e cient,and readily available electrocatalysts have been the focus for promoting the conversion of CO_(2). Very recently,interface engineering has been considered as a highly e ective strategy to modulate the electrocatalytic performance through electronic and/or structural modulation,regulations of electron/proton/mass/intermediates,and the control of local reactant concentration,thereby achieving desirable reaction pathway,inhibiting competing hydrogen generation,breaking binding-energy scaling relations of intermediates,and promoting CO_(2) mass transfer. In this review,we aim to provide a comprehensive overview of current developments in interface engineering for CO_(2) RR from both a theoretical and experimental stand-point,involving interfaces between metal and metal,metal and metal oxide,metal and nonmetal,metal oxide and metal oxide,organic molecules and inorganic materials,electrode and electrolyte,molecular catalysts and electrode,etc. Finally,the opportunities and challenges of interface engineering for CO_(2) RR are proposed.
基金funding support from 1000 Talent Plan program(NO.31370086963030)research projects from Shandong Province(2018JMRH0211,2017CXGC1010 and 2016GGX104001)+2 种基金Taishan Scholar Program(11370085961006)the National Science Foundation of Shandong Province(ZR2017MEM002)the Fundamental Research Funds of Shandong University(201810422046,2017JC010,2017JC042,and 2016JC005)。
文摘High ionic conductivity and superior interfacial stability of solid electrolytes at the electrodes are crucial factors for high-performance all-solid-state sodium batteries. Herein, a composite solid electrolyte Na3PS4-polyethylene oxide is synthesized by the solution-phase reaction method with an improved ionic conductivity up to 9.4 × 10-5 S/cm at room temperature. Moreover, polyethylene oxide polymer layer is wrapped homogeneously on the surface of Na3PS4 particles, which could effectively avoid the direct contact between Na3PS4 electrolyte and sodium metal, thus alleviate their side reactions. We demonstrate that all-solid-state battery SnS2/Na with the composite solid electrolyte Na3PS4-polyethylene oxide delivers an enhanced electrochemical performance with 230 m Ah/g after 40 cycles.
基金supported by funding from the Energy Materials and Surface Sciences Unit of the Okinawa Institute of Science and Technology Graduate Universitythe OIST R&D Cluster Research Program,the OIST Proof of Concept(POC)ProgramJST A-STEP Grant Number JPMJTM20HS,Japan。
文摘Tin dioxide(SnO_(2))has been demonstrated as one of the promising electron transport layers for high-efficiency perovskite solar cells(PSCs).However,scalable fabrication of SnO_(2) films with uniform coverage,desirable thickness and a low defect density in perovskite solar mod-ules(PSMs)is still challenging.Here,we report preparation of high-quality large-area SnO_(2) films by chemical bath depo-sition(CBD)with the addition of KMnO_(4).The strong oxidiz-ing nature of KMnO_(4) promotes the conversion from Sn(II)to Sn(VI),leading to reduced trap defects and a higher carrier mobility of SnO_(2).In addition,K ions diffuse into the per-ovskite film resulting in larger grain sizes,passivated grain boundaries,and reduced hysteresis of PSCs.Furthermore,Mn ion doping improves both the crystallinity and the phase stability of the perovskite film.Such a multifunctional interface engineering strategy enabled us to achieve a power conversion efficiency(PCE)of 21.70% with less hysteresis for lab-scale PSCs.Using this method,we also fabricated 5×5 and 10×10 cm^(2) PSMs,which showed PCEs of 15.62% and 11.80%(active area PCEs are 17.26%and 13.72%),respectively.For the encapsulated 5×5 cm^(2) PSM,we obtained a T80 operation lifetime(the lifespan during which the solar module PCE drops to 80%of its initial value)exceeding 1000 h in ambient condition.
基金supported by the National Natural Science Foundation of China (NSFC)(22075201)the National Key Research and Development Program of China (2022YFB4101800)。
文摘The electrochemical CO_(2)reduction reaction to produce multi-carbon(C_(2+)) hydrocarbons or oxygenate compounds is a promising route to obtain a renewable fuel of high energy density.However,producing C_(2+)at high current densities is still a challenge.Herein,we develop a Cu-Zn alloy/Cu-Zn aluminate oxide composite electrocatalytic system for enhanced conversion of CO_(2)to C_(2+)products.The Cu-Zn-Al-Layered Double Hydroxide(LDH) is used as a precursor to decompose into uniform Cu-Zn oxide/Cu-Zn aluminate pre-catalyst.Under electrochemical reduction,Cu-Zn oxide generates Cu-Zn alloy while Cu-Zn aluminate oxide remains unchanged.The alloy and oxide are closely stacked and arranged alternately,and the aluminate oxide induces the strong electron interaction of Cu,Zn and Al,creating a large number of highly active reaction interfaces composed of 0 to+3 valence metal sites.With the help of the interface effect,the optimized Cu_(9)Zn_(1)/Cu_(0.8)Zn_(0.2)Al_(2)O_(4)catalyst achieves a Faradaic efficiency of 88.5% for C_(2+)products at a current density of 400 mA cm^(-2)at-1.15 V versus reversible hydrogen electrode.The in-situ Raman and attenuate total reflectance-infrared absorption spectroscopy(ATR-IRAS) spectra show that the aluminate oxide at the interface significantly enhances the adsorption and activation of CO_(2)and the dissociation of H2O and strengthens the adsorption of CO intermediates,and the alloy promotes the C-C coupling to produce C_(2+)products.This work provides an efficient strategy to construct highly active reaction interfaces for industrial-scale electrochemical CO_(2)RR.
