The accumulation of multiple surface holes is considered to be the key to efficient photoelectrochemical(PEC)water oxidation.Previous PEC water oxidation studies commonly apply high potentials(>1.2 VRHE)to achieve ...The accumulation of multiple surface holes is considered to be the key to efficient photoelectrochemical(PEC)water oxidation.Previous PEC water oxidation studies commonly apply high potentials(>1.2 VRHE)to achieve this key.But how to complete multi-hole transfer under low bias(<1.2 VRHE)remains unknown.Herein,we find that,on a typical visible-light photoanode,hematite(α-Fe_(2)O_(3)),UV excitation plays a indispensable role in driving multi-hole water oxidation under low bias.Compared with the visible-light excitation,the UV excitation promotes the formation of adjacent surface-trapped holes onα-Fe_(2)O_(3) at 0.9VRHE,thereby increasing the reaction order of surface holes from~1 to~2 and improving the PEC water oxidation activity by one order of magnitude.The UV irradiation reduces the formation probability of self-trapped excitons and results in~3 to 5-fold increase of surface holes.These advantages enable the UV excitation to contribute about 40%to the total photocurrent under 1 solar illumination,even though its energy only occupies 6%of the incident light.This mechanism is also applicable to boost selective two-hole oxidation of thioether at 0.1 VFc/Fc+and nitrite at 0.9 VRHE.展开更多
As a promising graphene analogue,two-dimensional(2D)polymer nanosheets with unique 2D features,diversified topological structures and as well as tunable electronic properties,have received extensive attention in recen...As a promising graphene analogue,two-dimensional(2D)polymer nanosheets with unique 2D features,diversified topological structures and as well as tunable electronic properties,have received extensive attention in recent years.Here in this review,we summarized the recent research progress in the preparation methods of 2D polymer nanosheets,mainly including interfacial polymerization and solution polymerization.We also discussed the recent research advancements of 2D polymer nanosheets in the fields of energy storage and conversion applications,such as batteries,supercapacitors,electrocatalysis and photocatalysis.Finally,on the basis of their current development,we put forward the existing challenges and some personal perspectives.展开更多
Increasing concerns over climate change and energy shortage have driven the development of clean energy devices such as batteries,supercapacitors,fuel cells and solar water splitting in the past decades.And among pote...Increasing concerns over climate change and energy shortage have driven the development of clean energy devices such as batteries,supercapacitors,fuel cells and solar water splitting in the past decades.And among potential device materials,3D hierarchical carbon-rich micro-/nanomaterials(3D HCMNs)have come under intense scrutiny because they can prevent the stacking and bundling of low-dimensional building blocks to not only shorten diffusion distances for matter and charge to achieve high-energy-high-power storage but also greatly expose active sites to achieve highly active,durable and efficient catalysis.Based on this,this review will summarize the synthetic strategies and formation mechanisms of 3D HCMNs,including 3D nanocarbons,polymers,COFs/MOFs,templated carbons and derived carbon-based hybrids with a focus on 3D superstructures such as urchins,flowers,hierarchical tubular structures as well as nanoarrays including nanotube,nanofiber and nanosheet arrays.This review will also discuss the application of 3D HCMNs in energy storage and catalysis systems,including batteries,supercapacitors,electrocatalysis and photo(electro)catalysis.Overall,this review will provide a comprehensive overview of the recent progress of 3D HCMNs in terms of preparation strategies,formation mechanisms,structural diversities and electrochemical applications to provide a guideline for the rational design and structure–function exploration of 3D hierarchical nanomaterials from different sources beyond carbon-based species.展开更多
Vacancy engineering in metal sulfides has garnered enormous attention from researchers because of their outstanding ability to modulate the optical and physiochemical properties of photocatalysts.Typically,in the case...Vacancy engineering in metal sulfides has garnered enormous attention from researchers because of their outstanding ability to modulate the optical and physiochemical properties of photocatalysts.Typically,in the case of sulfides,the catalytic activity is drastically hindered by the quick reassembly of excitons and the photocorrosion effect.Hence designing and generating S-vacancies in metal sulfides has emerged as a potential strategy for attaining adequate water splitting to generate H_(2) and O_(2) because of the simulta-neous improvement in the optoelectronic features.However,developing efficient catalysts that manifest optimal photo(electro)catalytic performance for large-scale applicability remains challenging.Therefore,it is of utmost interest to explore the insightful features of creating S-vacancy and study their impact on catalytic performance.This review article aims to comprehensively highlight the roles of S-vacancy in sulfides for amended overall water-splitting activity.The photocatalytic features of S-vacancies modulated metal sulfides are deliberated,followed by various advanced synthetic and characterization techniques for effectual generation and identification of vacancy defects.The specific aspects of S-vacancies in refin-ing the optical absorption range charge carrier dynamics,and photoinduced surface chemical reactions are critically examined for overall water splitting applications.Finally,the vouchsafing outlooks and op-portunities confronting the defect-engineered(S-vacancy)metal sulfides-based photocatalysts have been summarized.展开更多
Wastewater management and energy/resource recycling have been extensively investigated via photo(electro)catalysis.Although both operation processes are driven effectively by the same interfacial charge,each system is...Wastewater management and energy/resource recycling have been extensively investigated via photo(electro)catalysis.Although both operation processes are driven effectively by the same interfacial charge,each system is practiced separately since they require very different reaction conditions.In this review,we showcase the recent advancements in photo(electro)catalytic process that enables the wastewater treatment and simultaneous energy/resource recovery(WT-ERR).Various literatures based on photo(electro)catalysis for wastewater treatment coupled with CO_(2)conversion,H_(2)production and heavy metal recovery are summarized.Besides,the fundamentals of photo(electro)catalysis and the influencing factors in such synergistic process are also presented.The essential feature of the catalysis lies in effectively utilizing hole oxidation for pollutant degradation and electron reduction for energy/resource recovery.Although in its infancy,the reviewed technology provides new avenue for developing next-generation wastewater treatment process.Moreover,we expect that this review can stimulate intensive researches to rationally design photo(electro)catalytic systems for environmental remediation accompanied with energy and resource recovery.展开更多
The photo-electro-catalytic oxidation of methanol in acid solution on Pt-Ru modified and unmodified titanium dioxide film electrodes has been studied. The photo-catalysis current of the OTE/TiO2 electrode and photo-el...The photo-electro-catalytic oxidation of methanol in acid solution on Pt-Ru modified and unmodified titanium dioxide film electrodes has been studied. The photo-catalysis current of the OTE/TiO2 electrode and photo-electro-catalysis current of the OTE/TiO2/Pt-Ru electrode both were three order of magnitude larger than that created by the common electrical oxidation. In addition, the effect of Pt-Ru on the current is described. The electrode sensitized by RuL2（NCS）2 showed a broader photoresponse spectral region.展开更多
Carbon nanotubes and graphene are carbon-based materials, which possess not only unique structure but also prop- erties such as high surface area, extraordinary mechanical properties, high electronic conductivity, and...Carbon nanotubes and graphene are carbon-based materials, which possess not only unique structure but also prop- erties such as high surface area, extraordinary mechanical properties, high electronic conductivity, and chemical stability. Thus, they have been regarded as an important material, especially for exploring a variety of complex catalysts. Considerable efforts have been made to functionalize and fabricate carbon-based composites with metal nanoparticles. In this review, we summarize the recent progress of our research on the decoration of carbon nanotubes/graphene with metal nanoparticles by using polyoxometalates as key agents, and their enhanced photo-electrical catalytic activities in various catalytic reactions. The polyoxometalates play a key role in constructing the nanohybrids and contributing to their photo-electrical catalytic properties.展开更多
A new type of photo-electro-chemical catalytic reactor was designed.Cathode and anode of the new reactor were made of high-purity graphite and titanium dioxide electrode re-spectively.A saturated calomel electrode (SC...A new type of photo-electro-chemical catalytic reactor was designed.Cathode and anode of the new reactor were made of high-purity graphite and titanium dioxide electrode re-spectively.A saturated calomel electrode (SCE) was used as the reference electrode.Under the condition of ultraviolet radiation and anodic bias-voltage,acid scarlet 3R was degraded by the process of photoelectrocatalysis with titanium dioxide electrode in anodic compartment,while it was degraded by electrogenerated Fenton’s reagent and hydrogen peroxide through reducing dissolved oxygen with graphite electrode in catholyte.The new reactor made the best use of photogenerated holes and photogenerated charge on the anode of the new reactor,which achieved the purpose of degrading acid scarlet 3R in the cathodic and anodic compartments simultaneously,i.e.“two electrodes and double effect”.The experimental results showed that,compared with other photoelectrocatalysis reactors (“two electrodes and single effect” reactor),the new reactor has obviously enhanced the degradation of acid scarlet 3R dye.With the con-centration of the dye being 30 mg·L?1 in water,under the operating conditions that when the inert supporting electrolyte concentration was 0.02 mol·L?1 sodium sulfate,initial solution pH = 3,and cathodic potential ?Ec = 0.66 V,the highest decolorizing efficiency of 92% was accomplished in cathodic compartment,and that of 60% in anodic compartment.展开更多
Efficient utilization of biomass for the supply of energy and synthetic materials would mitigate the heavy reliance on fossil resources and the growing CO_(2) emission, thus contributing to establishing sustainable an...Efficient utilization of biomass for the supply of energy and synthetic materials would mitigate the heavy reliance on fossil resources and the growing CO_(2) emission, thus contributing to establishing sustainable and carbon–neutral societies. Much effort has been devoted to catalytic transformations of lignocellulosic biomass, the most abundant and nonedible form of biomass.展开更多
针对染料废水净化问题,制得光催化材料MoS 2,并负载于碳刷上作为阴极,产电微生物作为阳极,构建产电微生物耦合光催化燃料电池系统,降解染料废水罗丹明B(RhB)的同时产生电能.通过调节光催化剂的负载量、电解质浓度、RhB浓度和光照条件等...针对染料废水净化问题,制得光催化材料MoS 2,并负载于碳刷上作为阴极,产电微生物作为阳极,构建产电微生物耦合光催化燃料电池系统,降解染料废水罗丹明B(RhB)的同时产生电能.通过调节光催化剂的负载量、电解质浓度、RhB浓度和光照条件等探究污染物的最佳降解条件.研究发现,电极负载0.1 g MoS 2且Na 2SO 4浓度为0.3 mol/L时,10 mg/L的RhB在黑暗条件下降解率可达99%.产电微生物耦合光催化燃料电池系统可不利用外加光源降解污染物,且降解过程中能够产生电能.展开更多
基金supported by the National Natural Science Foundation of China(22072158)the National Key R&D Program of China(2022YFA1505000,2020YFC1808401)+1 种基金the Strategic Priority Research Program of Chinese Academy of Sciences(XDB36000000)CAS Project for Young Scientists in Basic Research(YSBR-004).
文摘The accumulation of multiple surface holes is considered to be the key to efficient photoelectrochemical(PEC)water oxidation.Previous PEC water oxidation studies commonly apply high potentials(>1.2 VRHE)to achieve this key.But how to complete multi-hole transfer under low bias(<1.2 VRHE)remains unknown.Herein,we find that,on a typical visible-light photoanode,hematite(α-Fe_(2)O_(3)),UV excitation plays a indispensable role in driving multi-hole water oxidation under low bias.Compared with the visible-light excitation,the UV excitation promotes the formation of adjacent surface-trapped holes onα-Fe_(2)O_(3) at 0.9VRHE,thereby increasing the reaction order of surface holes from~1 to~2 and improving the PEC water oxidation activity by one order of magnitude.The UV irradiation reduces the formation probability of self-trapped excitons and results in~3 to 5-fold increase of surface holes.These advantages enable the UV excitation to contribute about 40%to the total photocurrent under 1 solar illumination,even though its energy only occupies 6%of the incident light.This mechanism is also applicable to boost selective two-hole oxidation of thioether at 0.1 VFc/Fc+and nitrite at 0.9 VRHE.
基金the National Natural Science Foundation of China(Nos.51873039 and 51673042)the Young Elite Scientist Sponsorship Program by CAST(No.2017QNRC001)the fund for post-doctoral program of Henan University to Z.H.C.(No.FJ3050A0670001).
文摘As a promising graphene analogue,two-dimensional(2D)polymer nanosheets with unique 2D features,diversified topological structures and as well as tunable electronic properties,have received extensive attention in recent years.Here in this review,we summarized the recent research progress in the preparation methods of 2D polymer nanosheets,mainly including interfacial polymerization and solution polymerization.We also discussed the recent research advancements of 2D polymer nanosheets in the fields of energy storage and conversion applications,such as batteries,supercapacitors,electrocatalysis and photocatalysis.Finally,on the basis of their current development,we put forward the existing challenges and some personal perspectives.
基金the Natural Sciences and Engineering Research Council of Canada(NSERC)through the Discovery Grant Program(RGPIN-2018-06725)the Discovery Accelerator Supplement Grant Program(RGPAS-2018-522651)the New Frontiers in Research Fund-Exploration Program(NFRFE-2019-00488).
文摘Increasing concerns over climate change and energy shortage have driven the development of clean energy devices such as batteries,supercapacitors,fuel cells and solar water splitting in the past decades.And among potential device materials,3D hierarchical carbon-rich micro-/nanomaterials(3D HCMNs)have come under intense scrutiny because they can prevent the stacking and bundling of low-dimensional building blocks to not only shorten diffusion distances for matter and charge to achieve high-energy-high-power storage but also greatly expose active sites to achieve highly active,durable and efficient catalysis.Based on this,this review will summarize the synthetic strategies and formation mechanisms of 3D HCMNs,including 3D nanocarbons,polymers,COFs/MOFs,templated carbons and derived carbon-based hybrids with a focus on 3D superstructures such as urchins,flowers,hierarchical tubular structures as well as nanoarrays including nanotube,nanofiber and nanosheet arrays.This review will also discuss the application of 3D HCMNs in energy storage and catalysis systems,including batteries,supercapacitors,electrocatalysis and photo(electro)catalysis.Overall,this review will provide a comprehensive overview of the recent progress of 3D HCMNs in terms of preparation strategies,formation mechanisms,structural diversities and electrochemical applications to provide a guideline for the rational design and structure–function exploration of 3D hierarchical nanomaterials from different sources beyond carbon-based species.
基金This research was supported by Brain Pool Program through the National Research Foundation of Korea(NRF)funded by the Ministry of Science and ICT(No.2020H1D3A1A04081409。
文摘Vacancy engineering in metal sulfides has garnered enormous attention from researchers because of their outstanding ability to modulate the optical and physiochemical properties of photocatalysts.Typically,in the case of sulfides,the catalytic activity is drastically hindered by the quick reassembly of excitons and the photocorrosion effect.Hence designing and generating S-vacancies in metal sulfides has emerged as a potential strategy for attaining adequate water splitting to generate H_(2) and O_(2) because of the simulta-neous improvement in the optoelectronic features.However,developing efficient catalysts that manifest optimal photo(electro)catalytic performance for large-scale applicability remains challenging.Therefore,it is of utmost interest to explore the insightful features of creating S-vacancy and study their impact on catalytic performance.This review article aims to comprehensively highlight the roles of S-vacancy in sulfides for amended overall water-splitting activity.The photocatalytic features of S-vacancies modulated metal sulfides are deliberated,followed by various advanced synthetic and characterization techniques for effectual generation and identification of vacancy defects.The specific aspects of S-vacancies in refin-ing the optical absorption range charge carrier dynamics,and photoinduced surface chemical reactions are critically examined for overall water splitting applications.Finally,the vouchsafing outlooks and op-portunities confronting the defect-engineered(S-vacancy)metal sulfides-based photocatalysts have been summarized.
基金financially supported by the National Natural Science Foundation of China(Nos.52000097,51878325,51868050 and 51938007)the Natural Science Foundation of Jiangxi Province(Nos.20192BAB213011 and 20192ACBL21046)+1 种基金the Ph.D.research startup foundation of Nanchang Hangkong University(No.EA201802367)the Open Project Program of the State Key Laboratory of Photocatalysis on Energy and Environment(No.SKLPEE-KF202106),Fuzhou University。
文摘Wastewater management and energy/resource recycling have been extensively investigated via photo(electro)catalysis.Although both operation processes are driven effectively by the same interfacial charge,each system is practiced separately since they require very different reaction conditions.In this review,we showcase the recent advancements in photo(electro)catalytic process that enables the wastewater treatment and simultaneous energy/resource recovery(WT-ERR).Various literatures based on photo(electro)catalysis for wastewater treatment coupled with CO_(2)conversion,H_(2)production and heavy metal recovery are summarized.Besides,the fundamentals of photo(electro)catalysis and the influencing factors in such synergistic process are also presented.The essential feature of the catalysis lies in effectively utilizing hole oxidation for pollutant degradation and electron reduction for energy/resource recovery.Although in its infancy,the reviewed technology provides new avenue for developing next-generation wastewater treatment process.Moreover,we expect that this review can stimulate intensive researches to rationally design photo(electro)catalytic systems for environmental remediation accompanied with energy and resource recovery.
文摘The photo-electro-catalytic oxidation of methanol in acid solution on Pt-Ru modified and unmodified titanium dioxide film electrodes has been studied. The photo-catalysis current of the OTE/TiO2 electrode and photo-electro-catalysis current of the OTE/TiO2/Pt-Ru electrode both were three order of magnitude larger than that created by the common electrical oxidation. In addition, the effect of Pt-Ru on the current is described. The electrode sensitized by RuL2（NCS）2 showed a broader photoresponse spectral region.
基金Project supported by the National Natural Science Foundation of China(Grant No.21371173)the National Basic Research Program of China(973 Program)(Grant No.2012CB932504)
文摘Carbon nanotubes and graphene are carbon-based materials, which possess not only unique structure but also prop- erties such as high surface area, extraordinary mechanical properties, high electronic conductivity, and chemical stability. Thus, they have been regarded as an important material, especially for exploring a variety of complex catalysts. Considerable efforts have been made to functionalize and fabricate carbon-based composites with metal nanoparticles. In this review, we summarize the recent progress of our research on the decoration of carbon nanotubes/graphene with metal nanoparticles by using polyoxometalates as key agents, and their enhanced photo-electrical catalytic activities in various catalytic reactions. The polyoxometalates play a key role in constructing the nanohybrids and contributing to their photo-electrical catalytic properties.
基金the Scientific and Technical Planned Project of Guangdong Province(Grant No.2002C31622) the Natural Science Foundation of Guangdong Province(Grant No.31921).
文摘A new type of photo-electro-chemical catalytic reactor was designed.Cathode and anode of the new reactor were made of high-purity graphite and titanium dioxide electrode re-spectively.A saturated calomel electrode (SCE) was used as the reference electrode.Under the condition of ultraviolet radiation and anodic bias-voltage,acid scarlet 3R was degraded by the process of photoelectrocatalysis with titanium dioxide electrode in anodic compartment,while it was degraded by electrogenerated Fenton’s reagent and hydrogen peroxide through reducing dissolved oxygen with graphite electrode in catholyte.The new reactor made the best use of photogenerated holes and photogenerated charge on the anode of the new reactor,which achieved the purpose of degrading acid scarlet 3R in the cathodic and anodic compartments simultaneously,i.e.“two electrodes and double effect”.The experimental results showed that,compared with other photoelectrocatalysis reactors (“two electrodes and single effect” reactor),the new reactor has obviously enhanced the degradation of acid scarlet 3R dye.With the con-centration of the dye being 30 mg·L?1 in water,under the operating conditions that when the inert supporting electrolyte concentration was 0.02 mol·L?1 sodium sulfate,initial solution pH = 3,and cathodic potential ?Ec = 0.66 V,the highest decolorizing efficiency of 92% was accomplished in cathodic compartment,and that of 60% in anodic compartment.
基金support by the National Key R&D Program of China(2018YFB1501602)the National Natural Science Foundation of China(22121001 and 22172127)。
文摘Efficient utilization of biomass for the supply of energy and synthetic materials would mitigate the heavy reliance on fossil resources and the growing CO_(2) emission, thus contributing to establishing sustainable and carbon–neutral societies. Much effort has been devoted to catalytic transformations of lignocellulosic biomass, the most abundant and nonedible form of biomass.
文摘针对染料废水净化问题,制得光催化材料MoS 2,并负载于碳刷上作为阴极,产电微生物作为阳极,构建产电微生物耦合光催化燃料电池系统,降解染料废水罗丹明B(RhB)的同时产生电能.通过调节光催化剂的负载量、电解质浓度、RhB浓度和光照条件等探究污染物的最佳降解条件.研究发现,电极负载0.1 g MoS 2且Na 2SO 4浓度为0.3 mol/L时,10 mg/L的RhB在黑暗条件下降解率可达99%.产电微生物耦合光催化燃料电池系统可不利用外加光源降解污染物,且降解过程中能够产生电能.
文摘在光/电/化学协同催化反应器中,以离子交换膜代替盐桥连通阴、阳两室,以30 mg/L的甲基红溶液为目标降解物,考察了不同连通方式、初始pH和阴极电位对反应的影响.结果表明:甲基红在阳离子膜型反应器中的表观反应速率常数明显高于盐桥型及阴离子交换膜型反应器,这是由于阳离子交换膜可以及时有效地将阳极室中产生的H+转移至阴极室中参与阴极反应.甲基红在阳离子膜型反应器中的去除率随溶液初始pH的增高而降低,随阴极电位的增加先增大后减小,最佳反应条件为pH=2.0～3.0,阴极电位(-Ec)=0.6 V.
