Peroxymonosulfate(PMS)is commonly used in advanced oxidation processes to degrade organic pollutants in wastewater.In this work,to obtain better PMS activation efficiency,Bi_(4)O_(5)Br_(2)/BCZT(BBT)piezoelectric photo...Peroxymonosulfate(PMS)is commonly used in advanced oxidation processes to degrade organic pollutants in wastewater.In this work,to obtain better PMS activation efficiency,Bi_(4)O_(5)Br_(2)/BCZT(BBT)piezoelectric photocatalyst was designed.Abundant active radicals produced by BBT under visible light irradiation and ultrasonic vibration were used to activate PMS,thereby achieving rapid degradation of high concentration pollutants.With the introduction of BCZT,the catalyst has a strong internal electric field and three-dimensional lamellar structure,which promotes the separation and transfer of electrons and holes.It is worth noting that under optimal reaction conditions,the degradation rate of ARB reached 93%by BBT15 within 10 min.The catalytic experiment combined with the piezoelectric performance test results revealed the key role of piezoelectric photocatalytic reaction in PMS activation.This provides an important prospect for PMS to effectively deal with the degradation of high concentrations of organic pollutants.展开更多
One key strategy to enhance photocatalytic performance is to improve the transfer and separation efficiency of photogenerated carriers by building optimized heterojunctions.Herein,novel Bi_(4)O_5Br_(2)/NH_(2)-MIL-125(...One key strategy to enhance photocatalytic performance is to improve the transfer and separation efficiency of photogenerated carriers by building optimized heterojunctions.Herein,novel Bi_(4)O_5Br_(2)/NH_(2)-MIL-125(Ti)Z-scheme heterojunctions are fabricated and used as photocatalysts for organic pollutant photodegradation.The NH_(2)-MIL-125(Ti)nanosheets are exfoliated via a self-developed alkali solution stripping approach and then uniformly decorated on Bi_(4)O_(5)Br_(2).The as-prepared Bi_(4)O_(5)Br_(2)/NH_(2)-MIL-125(Ti)presents more than 90%degradation of various pollutants,outperforming the counterpart individual ones.The various characterization results suggest that the enhanced degradation rate is due to the more intimate face-to-face interfacial contact of the lamellar Z-scheme heterojunction materials,in which the migration path of carriers from the material's interior to the surface can be reduced,in turn enhancing migration efficiency and separation capability significantly.A possible photocatalytic reaction mechanism is proposed based on the photoelectric behaviors,radical trapping experiments and liquid chromatography mass spectrometry analysis.This work promotes the development of new photocatalytic materials for heterojunctions with face-to-face interfacial contacts,as well as the effective purification of wastewater in environmental remediation.展开更多
Spin engineering is recognized as a promising strategy that modulates the association between d‐orbital electrons and the oxygenated species,and enhances the catalytic kinetics.However,few efforts have been made to c...Spin engineering is recognized as a promising strategy that modulates the association between d‐orbital electrons and the oxygenated species,and enhances the catalytic kinetics.However,few efforts have been made to clarify whether spin engineering could make a considerable enhancement for electrocatalytic water oxidation.Herein,we report the spin engineering of a nanocage‐structured(Co,Ni)Se_(2)/C@FeOOH,that showed significant oxygen evolution reaction(OER)activity.Magnetization measurement presented that the(Co,Ni)Se_(2)/C@FeOOH sample possesses higher polarization spin number(μb=6.966μB/f.u.)compared with that of the(Co,Ni)Se_(2)/C sample(μb=6.398μB/f.u.),for which the enlarged spin polarization number favors the adsorption and desorption energy of the intermediate oxygenated species,as confirmed by surface valance band spectra.Consequently,the(Co,Ni)Se_(2)/C@FeOOH affords remarkable OER product with a low overpotential of 241 mV at a current of 10 mA cm^(-2) and small Tafel slope of 44 mV dec^(-1) in 1.0 mol/L KOH alkaline solution,significantly surpassing the parent(Co,Ni)Se_(2)/C catalyst.This work will trigger a solid step for the design of highly‐efficient OER electrocatalysts.展开更多
The photocatalytic performance of g-C_(3)N_(4) for CO_(2) conversion is still inadequate by several shortfalls including the instability,insu cient solar light absorption and rapid charge carrier's recombination r...The photocatalytic performance of g-C_(3)N_(4) for CO_(2) conversion is still inadequate by several shortfalls including the instability,insu cient solar light absorption and rapid charge carrier's recombination rate. To solve these problems,herein,noble metals(Pt and Au)decorated Sr-incorporated g-C_(3)N_(4) photocatalysts are fabricated via the simple calcination and photo-deposition methods. The Sr-incorporation remarkably reduced the g-C_(3)N_(4) band gap from 2.7 to 2.54 eV,as evidenced by the UV–visible absorption spectra and the density functional theory results. The CO_(2) conversion performance of the catalysts was evaluated under visible light irradiation. The Pt/0.15 Sr-CN sample produced 48.55 and 74.54 μmol h-1 g-1 of CH_(4) and CO,respectively.These amounts are far greater than that produced by the Au/0.15 Sr-CN,0.15 Sr-CN,and CN samples. A high quantum e ciency of 2.92% is predicted for the Pt/0.15 Sr-CN sample. Further,the stability of the photocatalyst is confirmed via the photocatalytic recyclable test. The improved CO_(2) conversion performance of the catalyst is accredited to the promoted light absorption and remarkably enhanced charge separation via the Sr-incorporated mid gap states and the localized surface plasmon resonance e ect induced by noble metal nanoparticles.This work will provide a new approach for promoting the catalytic e ciency of g-C_(3)N_(4) for e cient solar fuel production.展开更多
Clean energy and a sustainable environment are grand challenges that the world is facing which can be addressed by converting solar energy into transportable and storable fuels(chemical fuel).The main scientific and t...Clean energy and a sustainable environment are grand challenges that the world is facing which can be addressed by converting solar energy into transportable and storable fuels(chemical fuel).The main scientific and technological challenges for efficient solar energy conversion,energy storage,and environmental applications are the stability,durability,and performance of low-cost functional materials.Among different nanomaterials,perovskite type LaFeO_(3)has been extensively investigated as a photocatalyst due to its abundance,high stability,compositional and structural fexibility,high electrocatalytic activity,efficient sunlight absorption,and tunable band gap and band edges.Hence,it is urgent to write a comprehensive review to highlight the trend,challenges,and prospects of LaFeO_(3)in the field of photocatalytic solar energy conversion and environment purification.This critical review summarizes the history and basic principles of photocatalysis.Further,it reviews in detail the LaFeO_(3),applications,shortcomings,and activity enhancement strategies including the design of nanostructures,elemental doping,and heterojunctions construction such as Type-I,Type-II,Z-Type,and uncommon heterojunctions.Besides,the optical and electronic properties,charge carriers separation,electron transport phenomenon and alignment of the band gaps in LaFeO_(3)-based heterostructures are comprehensively discussed.展开更多
A typical Z-scheme system is composed of two photocatalysts which generate two sets of charge carriers and split water into H2 and O2 at different locations.Scientists are struggling to enhance the efficiencies of the...A typical Z-scheme system is composed of two photocatalysts which generate two sets of charge carriers and split water into H2 and O2 at different locations.Scientists are struggling to enhance the efficiencies of these systems by maximizing their light absorption,engineering more stable redox couples,and discovering new O2 and H2 evolutions co-catalysts.In this work,Au decorated WO3/g-C3N4 Z-scheme nanocomposites are fabricated via wet-chemical and photo-deposition methods.The nanocomposites are utilized in photocatalysis for H2 production and 2,4-dichlorophenol(2,4-DCP)degradation.It is investigated that the optimized 4Au/6%WO3/CN nanocomposite is highly efficient for production of 69.9 and 307.3μmol h−1 g−1 H2 gas,respectively,under visible-light(λ>420 nm)and UV–visible illumination.Further,the fabricated 4Au/6%WO3/CN nanocomposite is significant(i.e.,100%degradation in 2 h)for 2,4-DCP degradation under visible light and highly stable in photocatalysis.A significant 4.17%quantum efficiency is recorded for H2 production at wavelength 420 nm.This enhanced performance is attributed to the improved charge separation and the surface plasmon resonance effect of Au nanoparticles.Solid-state density functional theory simulations are performed to countercheck and validate our experimental data.Positive surface formation energy,high charge transfer,and strong non-bonding interaction via electrostatic forces confirm the stability of 4Au/6%WO3/CN interface.展开更多
Achieving sustainable production and preventing further damage to natural resources and ecosystems is a critical and exciting area of debate,and a priority within the framework of the United Nations Sustainable Develo...Achieving sustainable production and preventing further damage to natural resources and ecosystems is a critical and exciting area of debate,and a priority within the framework of the United Nations Sustainable Development Goals(SDG12:Ensure sustainable consumption and production patterns)for food,water,and agriculture[1].Ensuring water sustainability as the cornerstone of sustainable development is essential for promoting social and economic progress,securing food security and ecosystem integrity,and sustaining human survival[2].Population growth,socio-economic development,and changing consumption patterns have increased global water consumption by approximately 1%per year over the past 40 years.As a result,global water scarcity has become increasingly severe,with the number of urban residents facing water shortages projected to rise from 930 million in 2016 to 1.7–2.4 billion by 2050[3].As reflected in global water consumption patterns,irrigated agriculture,food production,and feed cultivation account for approximately 70%of freshwater use[4].Hence,systematic planning of wastewater reuse for irrigation is particularly important,as treated wastewater reuse(WWR)is considered a promising alternative to freshwater resources.展开更多
With the expansion of distributed generation systems and demand response programs, the need to fully utilize distribution system capacity has increased. In addition, the potential bidirectional flow of power on distri...With the expansion of distributed generation systems and demand response programs, the need to fully utilize distribution system capacity has increased. In addition, the potential bidirectional flow of power on distribution networks demands voltage visibility and control at all voltage levels. Distribution system state estimations, however, have traditionally been less prioritized due to the lack of enough measurement points while being the major role player in knowing the real-time system states of active distribution networks. The advent of smart meters at LV loads, on the other hand, is giving relief to this shortcoming. This study explores the potential of bottom up load flow analysis based on customer level Automatic Meter Reading (AMRs) to compute short time forecasts of demands and distribution network system states. A state estimation frame-work, which makes use of available AMR data, is proposed and discussed.展开更多
To address the sluggish kinetics of the oxygen evolution reaction(OER),a potential approach is to rationally design and fabricate extremely effective single atom catalysts(SACs).Using an appropriate matrix to stabiliz...To address the sluggish kinetics of the oxygen evolution reaction(OER),a potential approach is to rationally design and fabricate extremely effective single atom catalysts(SACs).Using an appropriate matrix to stabilize single-atom active centers with optimal geometric and electronic structures is crucial for enhancing catalytic activity.Herein,we report the design and fabrication of Ir single atoms on NiFeZn layered double hydroxide(Ir-SAC/NiFeZn-LDH)electrocatalyst for highly efficient and stable OER.It is investigated that the NiFeZn support exhibits abundant defect sites and unsaturated coordination sites.These sites function to anchor and stabilize single Ir single atoms on the support.The strong synergetic electronic interaction between the Ir single atoms and the NiFeZn matrix resulted in remarkable OER performance of the as-fabricated Ir-SAC/NiFeZn catalyst.With a loading Ir content of 1.09 wt.%,this catalyst demonstrates a highly stable OER activity,with an overpotential of 196 mV at 10 mA·cm^(−2) and a small Tafel slope of 35 mV·dec^(−1) for the OER in a 1 M KOH solution.These results significantly surpass the performance of the commercially available IrO_(2) catalyst.展开更多
Highly active and low-cost oxygen evolution reaction(OER)catalytic electrodes are extremely essential for exploration of green hydrogen via water splitting.Herein,an advanced Fe-Ni-F electrocatalyst is fabricated by a...Highly active and low-cost oxygen evolution reaction(OER)catalytic electrodes are extremely essential for exploration of green hydrogen via water splitting.Herein,an advanced Fe-Ni-F electrocatalyst is fabricated by a facile annealing strategy using ammonium fluoride,of which the structure feature is unveiled by XRD,FESEM,TEM,EDS,BET,and XPS measurements.The as-prepared Fe-Ni-F addresses a low overpotential of 277 mV and a small Tafel slope of 49 mV dec^(-1)at a current density of 10 mA cm^(-2),significantly outperforming other control samples as well as the state-of-the-art RuO_(2).The advanced nature of our Fe-Ni-F catalyst could also be further evidenced from the robust stability in KOH alkaline solution,showing as 5.41%degradation after 24 h continuous working.Upon analysis,it suggests that the decent catalytic activity should be attributed to the formed bimetallic(oxy)hydroxides because of the introduction of fluoride and the synergistic effect of iron and nickel towards oxygen generation.This work represents the potential of Fe-and/or Ni-based fluoride as efficient catalyst for low-energy consumption oxygen generation.展开更多
The release of anthropogenic CO_(2)emissions into the atmosphere has significantly accelerated global warming within the past few decades.According to the latest data,it is predicted that the concentration of CO_(2)wi...The release of anthropogenic CO_(2)emissions into the atmosphere has significantly accelerated global warming within the past few decades.According to the latest data,it is predicted that the concentration of CO_(2)will rise to 800 ppm over this century,and could reach 2000 ppm by 2300.Such high level of CO_(2)is expected to result in significant increase in global temperature as well as ocean acidification[1].展开更多
Anodic urea oxidation reaction(UOR)is an intriguing half reaction that can replace oxygen evolution reaction(OER)and work together with hydrogen evolution reaction(HER)toward simultaneous hydrogen fuel generation and ...Anodic urea oxidation reaction(UOR)is an intriguing half reaction that can replace oxygen evolution reaction(OER)and work together with hydrogen evolution reaction(HER)toward simultaneous hydrogen fuel generation and urea-rich wastewater purification;however,it remains a challenge to achieve overall urea electrolysis with high efficiency.Herein,we report a multifunctional electrocatalyst termed as Rh/Ni V-LDH,through integration of nickel-vanadium layered double hydroxide(LDH)with rhodium single-atom catalyst(SAC),to achieve this goal.The electrocatalyst delivers high HER mass activity of0.262 A mg^(-1) and exceptionally high turnover frequency(TOF)of 2.125 s^(-1) at an overpotential of100 m V.Moreover,exceptional activity toward urea oxidation is addressed,which requires a potential of 1.33 V to yield 10 mA cm^(-2),endorsing the potential to surmount the sluggish OER.The splendid catalytic activity is enabled by the synergy of the Ni V-LDH support and the atomically dispersed Rh sites(located on the Ni-V hollow sites)as evidenced both experimentally and theoretically.The selfsupported Rh/Ni V-LDH catalyst serving as the anode and cathode for overall urea electrolysis(1 mol L^(-1) KOH with 0.33 mol L^(-1) urea as electrolyte)only requires a small voltage of 1.47 V to deliver 100 mA cm^(-2) with excellent stability.This work provides important insights into multifunctional SAC design from the perspective of support sites toward overall electrolysis applications.展开更多
Electrocatalytic urea oxidation reaction(UOR)is regarded as an effective yet challenging approach for the degradation of urea in wastewater into harmless N2 and CO_(2).To overcome the sluggish kinetics,catalytically a...Electrocatalytic urea oxidation reaction(UOR)is regarded as an effective yet challenging approach for the degradation of urea in wastewater into harmless N2 and CO_(2).To overcome the sluggish kinetics,catalytically active sites should be rationally designed to maneuver the multiple key steps of intermediate adsorption and desorption.Herein,we demonstrate that metal-organic frameworks(MOFs)can provide an ideal platform for tailoring binary active sites to facilitate the rate-determining steps,achieving remarkable electrocatalytic activity toward UOR.Specifically,the MOF(namely,NiMn_(0.14)-BDC)based on Ni/Mn sites and terephthalic acid(BDC)ligands exhibits a low voltage of 1.317 V to deliver a current density of 10 mA cm^(-2).As a result,a high turnover frequency(TOF)of 0.15 s^(-1) is achieved at a voltage of 1.4 V,which enables a urea degradation rate of 81.87%in 0.33 M urea solution.The combination of experimental characterization with theoretical calculation reveals that the Ni and Mn sites play synergistic roles in maneuvering the evolution of urea molecules and key reaction intermediates during the UOR,while the binary Ni/Mn sites in MOF offer the tunability for electronic structure and d-band center impacting on the intermediate evolution.This work provides important insights into active site design by leveraging MOF platform and represents a solid step toward highly efficient UOR with MOF-based electrocatalysts.展开更多
基金financially supported by the National Natural Science Foundation of China(No.51302061)Natural Science Foundation of Hebei Province(No.E2020201021 and E2023201019)+4 种基金Industry-University-Research Cooperation Major Projects of Shijiazhuang(No.241130477A)Research Innovation Team of College of Chemistry and Environmental Science of Hebei University(No.hxkytd2102)Industry-University-research Cooperation Project of Colleges and Universities in Hebei Province(No.CXZX2025016)Hebei Province Innovation Capability Enhancement Plan Project(No.22567620H)Bintuan Science and Technology Program(Nos.2020DB002 and 2022DB009)。
文摘Peroxymonosulfate(PMS)is commonly used in advanced oxidation processes to degrade organic pollutants in wastewater.In this work,to obtain better PMS activation efficiency,Bi_(4)O_(5)Br_(2)/BCZT(BBT)piezoelectric photocatalyst was designed.Abundant active radicals produced by BBT under visible light irradiation and ultrasonic vibration were used to activate PMS,thereby achieving rapid degradation of high concentration pollutants.With the introduction of BCZT,the catalyst has a strong internal electric field and three-dimensional lamellar structure,which promotes the separation and transfer of electrons and holes.It is worth noting that under optimal reaction conditions,the degradation rate of ARB reached 93%by BBT15 within 10 min.The catalytic experiment combined with the piezoelectric performance test results revealed the key role of piezoelectric photocatalytic reaction in PMS activation.This provides an important prospect for PMS to effectively deal with the degradation of high concentrations of organic pollutants.
基金financially supported by the National Natural Science Foundation of China(No.51302061)the Natural Science Foundation of Hebei province(Nos.E2014201076,E2020201021 and E2023201019)+3 种基金the Research Innovation Team of College of Chemistry and Environmental Science of Hebei University(No.hxkytd2102)Shenzhen Science and Technology Innovation Committee(No.JCYJ20200109141412308)Bintuan Science and Technology Program(Nos.2020DB002 and 2022DB009)CWO funding of Ghent University。
文摘One key strategy to enhance photocatalytic performance is to improve the transfer and separation efficiency of photogenerated carriers by building optimized heterojunctions.Herein,novel Bi_(4)O_5Br_(2)/NH_(2)-MIL-125(Ti)Z-scheme heterojunctions are fabricated and used as photocatalysts for organic pollutant photodegradation.The NH_(2)-MIL-125(Ti)nanosheets are exfoliated via a self-developed alkali solution stripping approach and then uniformly decorated on Bi_(4)O_(5)Br_(2).The as-prepared Bi_(4)O_(5)Br_(2)/NH_(2)-MIL-125(Ti)presents more than 90%degradation of various pollutants,outperforming the counterpart individual ones.The various characterization results suggest that the enhanced degradation rate is due to the more intimate face-to-face interfacial contact of the lamellar Z-scheme heterojunction materials,in which the migration path of carriers from the material's interior to the surface can be reduced,in turn enhancing migration efficiency and separation capability significantly.A possible photocatalytic reaction mechanism is proposed based on the photoelectric behaviors,radical trapping experiments and liquid chromatography mass spectrometry analysis.This work promotes the development of new photocatalytic materials for heterojunctions with face-to-face interfacial contacts,as well as the effective purification of wastewater in environmental remediation.
文摘Spin engineering is recognized as a promising strategy that modulates the association between d‐orbital electrons and the oxygenated species,and enhances the catalytic kinetics.However,few efforts have been made to clarify whether spin engineering could make a considerable enhancement for electrocatalytic water oxidation.Herein,we report the spin engineering of a nanocage‐structured(Co,Ni)Se_(2)/C@FeOOH,that showed significant oxygen evolution reaction(OER)activity.Magnetization measurement presented that the(Co,Ni)Se_(2)/C@FeOOH sample possesses higher polarization spin number(μb=6.966μB/f.u.)compared with that of the(Co,Ni)Se_(2)/C sample(μb=6.398μB/f.u.),for which the enlarged spin polarization number favors the adsorption and desorption energy of the intermediate oxygenated species,as confirmed by surface valance band spectra.Consequently,the(Co,Ni)Se_(2)/C@FeOOH affords remarkable OER product with a low overpotential of 241 mV at a current of 10 mA cm^(-2) and small Tafel slope of 44 mV dec^(-1) in 1.0 mol/L KOH alkaline solution,significantly surpassing the parent(Co,Ni)Se_(2)/C catalyst.This work will trigger a solid step for the design of highly‐efficient OER electrocatalysts.
基金financially supported by the Ministry of Science and Technology of China (Grant No. 2018YFA0702100)the National Natural Science Foundation of China (Grant No. 11874169,51972129)+4 种基金the National Key R&D Program of China (Grant No. 2017YFE0120500)the Key Research and Development Program of Hubei (Grant No. 2020BAB079)the South Xinjiang Innovation and Development Program of Key Industries of Xinjiang Production and Construction Corps (Grants No. 2020DB002)Engineering and Physical Sciences Research Council (EP/T025875/1)the Hubei “ChuTian Young Scholar” program。
文摘The photocatalytic performance of g-C_(3)N_(4) for CO_(2) conversion is still inadequate by several shortfalls including the instability,insu cient solar light absorption and rapid charge carrier's recombination rate. To solve these problems,herein,noble metals(Pt and Au)decorated Sr-incorporated g-C_(3)N_(4) photocatalysts are fabricated via the simple calcination and photo-deposition methods. The Sr-incorporation remarkably reduced the g-C_(3)N_(4) band gap from 2.7 to 2.54 eV,as evidenced by the UV–visible absorption spectra and the density functional theory results. The CO_(2) conversion performance of the catalysts was evaluated under visible light irradiation. The Pt/0.15 Sr-CN sample produced 48.55 and 74.54 μmol h-1 g-1 of CH_(4) and CO,respectively.These amounts are far greater than that produced by the Au/0.15 Sr-CN,0.15 Sr-CN,and CN samples. A high quantum e ciency of 2.92% is predicted for the Pt/0.15 Sr-CN sample. Further,the stability of the photocatalyst is confirmed via the photocatalytic recyclable test. The improved CO_(2) conversion performance of the catalyst is accredited to the promoted light absorption and remarkably enhanced charge separation via the Sr-incorporated mid gap states and the localized surface plasmon resonance e ect induced by noble metal nanoparticles.This work will provide a new approach for promoting the catalytic e ciency of g-C_(3)N_(4) for e cient solar fuel production.
基金financially supported by the Ministry of Science and Technology of China(Grant No.2018YFA0702100)the National Natural Science Foundation of China(Grant Nos.11874169,51972129)+3 种基金the National Key R&D Program of China(Grant No.2017YFE0120500)the Key Research and Development Program of Hubei(Grant No.2020BAB079)the South Xinjiang Innovation and Development Program of Key Industries of Xinjiang Production and Construction Corps(Grants No.2020DB002)the Hubei‘‘Chu-Tian Young Scholar”program.
文摘Clean energy and a sustainable environment are grand challenges that the world is facing which can be addressed by converting solar energy into transportable and storable fuels(chemical fuel).The main scientific and technological challenges for efficient solar energy conversion,energy storage,and environmental applications are the stability,durability,and performance of low-cost functional materials.Among different nanomaterials,perovskite type LaFeO_(3)has been extensively investigated as a photocatalyst due to its abundance,high stability,compositional and structural fexibility,high electrocatalytic activity,efficient sunlight absorption,and tunable band gap and band edges.Hence,it is urgent to write a comprehensive review to highlight the trend,challenges,and prospects of LaFeO_(3)in the field of photocatalytic solar energy conversion and environment purification.This critical review summarizes the history and basic principles of photocatalysis.Further,it reviews in detail the LaFeO_(3),applications,shortcomings,and activity enhancement strategies including the design of nanostructures,elemental doping,and heterojunctions construction such as Type-I,Type-II,Z-Type,and uncommon heterojunctions.Besides,the optical and electronic properties,charge carriers separation,electron transport phenomenon and alignment of the band gaps in LaFeO_(3)-based heterostructures are comprehensively discussed.
基金the National Natural Science Foundation of China (Nos. 11874169, 11574106, 61771448, and 51635007)the Double first-class research funding of China-EU Institute for Clean and Renewable Energy (ICARE-RP-2018-SOLAR-003)+1 种基金the Engineering and Physical Science Research Council, UK (EPSRC grant No EP/ P510956/1 and EP/R512801/1the China Postdoctoral Science Foundation under Grant No. 2017M622404
文摘A typical Z-scheme system is composed of two photocatalysts which generate two sets of charge carriers and split water into H2 and O2 at different locations.Scientists are struggling to enhance the efficiencies of these systems by maximizing their light absorption,engineering more stable redox couples,and discovering new O2 and H2 evolutions co-catalysts.In this work,Au decorated WO3/g-C3N4 Z-scheme nanocomposites are fabricated via wet-chemical and photo-deposition methods.The nanocomposites are utilized in photocatalysis for H2 production and 2,4-dichlorophenol(2,4-DCP)degradation.It is investigated that the optimized 4Au/6%WO3/CN nanocomposite is highly efficient for production of 69.9 and 307.3μmol h−1 g−1 H2 gas,respectively,under visible-light(λ>420 nm)and UV–visible illumination.Further,the fabricated 4Au/6%WO3/CN nanocomposite is significant(i.e.,100%degradation in 2 h)for 2,4-DCP degradation under visible light and highly stable in photocatalysis.A significant 4.17%quantum efficiency is recorded for H2 production at wavelength 420 nm.This enhanced performance is attributed to the improved charge separation and the surface plasmon resonance effect of Au nanoparticles.Solid-state density functional theory simulations are performed to countercheck and validate our experimental data.Positive surface formation energy,high charge transfer,and strong non-bonding interaction via electrostatic forces confirm the stability of 4Au/6%WO3/CN interface.
基金supported by the National Natural Science Foundation of China(52272202 and W2421027).
文摘Achieving sustainable production and preventing further damage to natural resources and ecosystems is a critical and exciting area of debate,and a priority within the framework of the United Nations Sustainable Development Goals(SDG12:Ensure sustainable consumption and production patterns)for food,water,and agriculture[1].Ensuring water sustainability as the cornerstone of sustainable development is essential for promoting social and economic progress,securing food security and ecosystem integrity,and sustaining human survival[2].Population growth,socio-economic development,and changing consumption patterns have increased global water consumption by approximately 1%per year over the past 40 years.As a result,global water scarcity has become increasingly severe,with the number of urban residents facing water shortages projected to rise from 930 million in 2016 to 1.7–2.4 billion by 2050[3].As reflected in global water consumption patterns,irrigated agriculture,food production,and feed cultivation account for approximately 70%of freshwater use[4].Hence,systematic planning of wastewater reuse for irrigation is particularly important,as treated wastewater reuse(WWR)is considered a promising alternative to freshwater resources.
文摘With the expansion of distributed generation systems and demand response programs, the need to fully utilize distribution system capacity has increased. In addition, the potential bidirectional flow of power on distribution networks demands voltage visibility and control at all voltage levels. Distribution system state estimations, however, have traditionally been less prioritized due to the lack of enough measurement points while being the major role player in knowing the real-time system states of active distribution networks. The advent of smart meters at LV loads, on the other hand, is giving relief to this shortcoming. This study explores the potential of bottom up load flow analysis based on customer level Automatic Meter Reading (AMRs) to compute short time forecasts of demands and distribution network system states. A state estimation frame-work, which makes use of available AMR data, is proposed and discussed.
基金supported by the National Key R&D Program of China(No.2021YFF0500500)National Natural Science Foundation of China(Nos.21925202 and U22B2071)+1 种基金Yunnan Provincial Science and Technology Project at Southwest United Graduate School(No.202302AO370017)International Joint Mission on Climate Change and Carbon Neutrality.
文摘To address the sluggish kinetics of the oxygen evolution reaction(OER),a potential approach is to rationally design and fabricate extremely effective single atom catalysts(SACs).Using an appropriate matrix to stabilize single-atom active centers with optimal geometric and electronic structures is crucial for enhancing catalytic activity.Herein,we report the design and fabrication of Ir single atoms on NiFeZn layered double hydroxide(Ir-SAC/NiFeZn-LDH)electrocatalyst for highly efficient and stable OER.It is investigated that the NiFeZn support exhibits abundant defect sites and unsaturated coordination sites.These sites function to anchor and stabilize single Ir single atoms on the support.The strong synergetic electronic interaction between the Ir single atoms and the NiFeZn matrix resulted in remarkable OER performance of the as-fabricated Ir-SAC/NiFeZn catalyst.With a loading Ir content of 1.09 wt.%,this catalyst demonstrates a highly stable OER activity,with an overpotential of 196 mV at 10 mA·cm^(−2) and a small Tafel slope of 35 mV·dec^(−1) for the OER in a 1 M KOH solution.These results significantly surpass the performance of the commercially available IrO_(2) catalyst.
基金supported by the National Natural Science Foundation of China(No.51804223,52272202)the Innovation Foundation of Key Laboratory of Green Chemical Process of Ministry of Education(No.GCX202113)+1 种基金Bintuan Science and Technology Program(No.2020DB002,2022DB009)the Shenzhen Science and Technology Innovation Committee(No.JCYJ20200109141412308).
文摘Highly active and low-cost oxygen evolution reaction(OER)catalytic electrodes are extremely essential for exploration of green hydrogen via water splitting.Herein,an advanced Fe-Ni-F electrocatalyst is fabricated by a facile annealing strategy using ammonium fluoride,of which the structure feature is unveiled by XRD,FESEM,TEM,EDS,BET,and XPS measurements.The as-prepared Fe-Ni-F addresses a low overpotential of 277 mV and a small Tafel slope of 49 mV dec^(-1)at a current density of 10 mA cm^(-2),significantly outperforming other control samples as well as the state-of-the-art RuO_(2).The advanced nature of our Fe-Ni-F catalyst could also be further evidenced from the robust stability in KOH alkaline solution,showing as 5.41%degradation after 24 h continuous working.Upon analysis,it suggests that the decent catalytic activity should be attributed to the formed bimetallic(oxy)hydroxides because of the introduction of fluoride and the synergistic effect of iron and nickel towards oxygen generation.This work represents the potential of Fe-and/or Ni-based fluoride as efficient catalyst for low-energy consumption oxygen generation.
基金supported by National Natural Science Foundation of China(Nos.51972129,52272202)the National Key R&D Program of China(No.2022YFB3807201)Bintuan Science and Technology Program(Nos.2020DB002,2022DB009).
文摘The release of anthropogenic CO_(2)emissions into the atmosphere has significantly accelerated global warming within the past few decades.According to the latest data,it is predicted that the concentration of CO_(2)will rise to 800 ppm over this century,and could reach 2000 ppm by 2300.Such high level of CO_(2)is expected to result in significant increase in global temperature as well as ocean acidification[1].
基金finically supported by the National Key R&D Program of China(2017YFE0120500)the National Natural Science Foundation of China(51972129,51702150,and 21725102)+2 种基金the Key Research and Development Program of Hubei(2020BAB079)Bintuan Science and Technology Program(2020DB002,and 2022DB009)the Science and Technology Innovation Committee Foundation of Shenzhen(JCYJ20210324141613032 and JCYJ20190809142019365)。
文摘Anodic urea oxidation reaction(UOR)is an intriguing half reaction that can replace oxygen evolution reaction(OER)and work together with hydrogen evolution reaction(HER)toward simultaneous hydrogen fuel generation and urea-rich wastewater purification;however,it remains a challenge to achieve overall urea electrolysis with high efficiency.Herein,we report a multifunctional electrocatalyst termed as Rh/Ni V-LDH,through integration of nickel-vanadium layered double hydroxide(LDH)with rhodium single-atom catalyst(SAC),to achieve this goal.The electrocatalyst delivers high HER mass activity of0.262 A mg^(-1) and exceptionally high turnover frequency(TOF)of 2.125 s^(-1) at an overpotential of100 m V.Moreover,exceptional activity toward urea oxidation is addressed,which requires a potential of 1.33 V to yield 10 mA cm^(-2),endorsing the potential to surmount the sluggish OER.The splendid catalytic activity is enabled by the synergy of the Ni V-LDH support and the atomically dispersed Rh sites(located on the Ni-V hollow sites)as evidenced both experimentally and theoretically.The selfsupported Rh/Ni V-LDH catalyst serving as the anode and cathode for overall urea electrolysis(1 mol L^(-1) KOH with 0.33 mol L^(-1) urea as electrolyte)only requires a small voltage of 1.47 V to deliver 100 mA cm^(-2) with excellent stability.This work provides important insights into multifunctional SAC design from the perspective of support sites toward overall electrolysis applications.
基金This work is finically supported by the National Key R&D Program of China(Grant No.2017YFE0120500)the National Natural Science Foundation of China(Grant Nos.51972129,21725102)+3 种基金the Bintuan Science and Technology Program(Grant Nos.2020DB002,2022DB009)the Key Research and Development Program of Hubei(Grant No.2020BAB079)the Science and Technology Innovation Committee Foundation of Shenzhen(Grant No.JCYJ20210324141613032)the Natural Science Foundation of Jiangsu Province of China(BK20211609).
文摘Electrocatalytic urea oxidation reaction(UOR)is regarded as an effective yet challenging approach for the degradation of urea in wastewater into harmless N2 and CO_(2).To overcome the sluggish kinetics,catalytically active sites should be rationally designed to maneuver the multiple key steps of intermediate adsorption and desorption.Herein,we demonstrate that metal-organic frameworks(MOFs)can provide an ideal platform for tailoring binary active sites to facilitate the rate-determining steps,achieving remarkable electrocatalytic activity toward UOR.Specifically,the MOF(namely,NiMn_(0.14)-BDC)based on Ni/Mn sites and terephthalic acid(BDC)ligands exhibits a low voltage of 1.317 V to deliver a current density of 10 mA cm^(-2).As a result,a high turnover frequency(TOF)of 0.15 s^(-1) is achieved at a voltage of 1.4 V,which enables a urea degradation rate of 81.87%in 0.33 M urea solution.The combination of experimental characterization with theoretical calculation reveals that the Ni and Mn sites play synergistic roles in maneuvering the evolution of urea molecules and key reaction intermediates during the UOR,while the binary Ni/Mn sites in MOF offer the tunability for electronic structure and d-band center impacting on the intermediate evolution.This work provides important insights into active site design by leveraging MOF platform and represents a solid step toward highly efficient UOR with MOF-based electrocatalysts.
基金the National Natural Science Foundation of China (No.11574106, 61771448and 51635007)the China Postdoctoral Science Foundation (No.2017M622404)and the Fundamental Research Projects of Shenzhen City (No.JCYJ20150831202835225).
