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
Sustainable and clean hydrogen development has been considered a mainstream trend in contemporary energy research.Heterogenous photo(electro)catalysis is a promising approach to producing hydrogen in an environmentall...Sustainable and clean hydrogen development has been considered a mainstream trend in contemporary energy research.Heterogenous photo(electro)catalysis is a promising approach to producing hydrogen in an environmentally friendly manner.Perovskites have emerged as an inexpensive,earth-abundant,and easily fabricated semiconductor material for photo(electro)catalysis.However,some of their shortcomings have limited the wide range of applications.In this mini-review,we present the fundamentals and applications of various perovskites for photo(electro)catalytic water splitting.In addition,we summarize advanced strategies for photo(electro)catalytic water splitting based on perovskites,focusing on the following approaches:intrinsic modulation of perovskites,functionalization of perovskites,and design of perovskite tandem systems.In summary,we point out the challenges and potential applications for perovskite solar water splitting and systematically describe various strategies to improve the photo(electro)catalysis performance of perovskites,illustrating the potential of using perovskites as key materials for solar water splitting.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
Efficient,stable,and noble‐metal‐free electrocatalysts for both the oxygen evolution reaction and the hydrogen evolution reaction are highly imperative for the realization of low‐cost commercial water‐splitting el...Efficient,stable,and noble‐metal‐free electrocatalysts for both the oxygen evolution reaction and the hydrogen evolution reaction are highly imperative for the realization of low‐cost commercial water‐splitting electrolyzers.Herein,a cost‐effective and ecofriendly strategy is reported to fabricate coral‐like FeNi(OH)x/Ni as a bifunctional electrocatalyst for overall water splitting in alkaline media.With the assistance of mild corrosion of Ni by Fe(NO3)3,in situ generated FeNi(OH)x nanosheets are intimately attached on metallic coral‐like Ni.Integration of these nanosheets with the electrodeposited coral‐like Ni skeleton and the supermacroporous Ni foam substrate forms a binder‐free hierarchical electrode,which is beneficial for exposing catalytic active sites,accelerating mass transport,and facilitating the release of gaseous species.In 1.0 mol L^-1 KOH solution,a symmetric electrolyzer constructed with FeNi(OH)x/Ni as both the anode and the cathode exhibits an excellent activity with an applied potential difference of 1.52 V at 10 mA cm^-2,which is superior to that of an asymmetric electrolyzer constructed with the state‐of‐the‐art RuO2‐PtC couple(applied potential difference of 1.55 V at 10 mA cm^-2).This work contributes a facile and reliable strategy for manufacturing affordable,practical,and promising water‐splitting devices.展开更多
The Ti base PbO 2 electrode prepared by electrodeposition of PbO 2 on the surface of titanium was used for electro catalytic oxidation of phenol in waste water. The experimental results show that the electrodeposition...The Ti base PbO 2 electrode prepared by electrodeposition of PbO 2 on the surface of titanium was used for electro catalytic oxidation of phenol in waste water. The experimental results show that the electrodeposition of PbO 2 at a higher current density for a short time, then followed by a lower current density can get a compact and combinative PbO 2 layer. The properties of a Ti/PbO 2 electrode with an interlayer of oxide are the best. When this kind of electrode is used to treat phenol containing waste water, the phenol removal rate is higher and the slot voltage is lower. In addition, by using the phenol removal rate as an index, the influences of electrolysis current density, mass transfer condition and pH were studied and the optimal condition was confirmed.展开更多
Photocatalytic membranes hold significant potential for promoting pollutant degradation and reducing membrane fouling in filtration systems.Although extensive research has been conducted on the independent design of p...Photocatalytic membranes hold significant potential for promoting pollutant degradation and reducing membrane fouling in filtration systems.Although extensive research has been conducted on the independent design of photocatalysts or membrane materials to improve their catalytic and filtration performance,the complex structures and interface mechanisms,as well as insufficient light utilization,are still often overlooked,limiting the overall performance improvement of photocatalytic membranes.This work provides an overview of enhancement strategies involving restricted area effects,external fields,such as mechanical,magnetic,thermal,and electrical fields,as well as coupling techniques with advanced oxidation processes(e.g.,O_(3),Fenton,and persulfate oxidation)for dual enhancement of photocatalysts and membranes.In addition,the synthesis method of photocatalytic membranes and the influence of factors,such as light source type,frequency,and relative position on photocatalytic membrane performance were also studied.Finally,economic feasibility and pollutant removal performance were further evaluated to determine the promising enhancement strategies,paving the way for more efficient and scalable applications of photocatalytic membranes.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
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
Reported here is a precise electro-reduction strategy for radical defluorinative alkylation towards the synthesis of gem-difluoroalkenes from α-trifluoromethylstyrenes. According to the redox-potential difference of ...Reported here is a precise electro-reduction strategy for radical defluorinative alkylation towards the synthesis of gem-difluoroalkenes from α-trifluoromethylstyrenes. According to the redox-potential difference of the radical precursors, direct or indirect electrolysis is respectively adopted to realize the precise reduction. An easy-to-handle, catalyst-and metal-free condition is developed for the reduction of alkyl radical precursors that are generally easier to be reduced than α-trifluoromethylstyrenes,while a novel electro-Ni-catalytic system is established for the electro-reduction of alkyl bromides or chlorides towards the electrochemical synthesis of gem-difluoroalkenes. The merit of this protocol is exhibited by its mild conditions, wide substrate scope, and scalable preparation. Mechanistic studies and DFT calculations proved that the coordination of α-trifluoromethylstyrenes to Ni-catalyst prevents the direct reduction of the alkene and, in turn, promotes the activation of alkyl bromide through halogen atom transfer mechanism.展开更多
Ammonia is a cornerstone of global agriculture and chemical manufacturing,with emerging potential as a carbon-free energy carrier.However,its conventional production via the Haber-Bosch process is energy-intensive,rel...Ammonia is a cornerstone of global agriculture and chemical manufacturing,with emerging potential as a carbon-free energy carrier.However,its conventional production via the Haber-Bosch process is energy-intensive,relies heavily on fossil fuels,and results in significant CO_(2) emissions.In pursuit of sustainable alternatives,renewable energy-driven synthesis routes have attracted growing interest.This review surveys recent advances in green ammonia production,covering electrocatalytic,photocatalytic,photo-electrocatalytic,and photothermal pathways,with an emphasis on the mechanistic understanding of nitrogen reduction from various feedstocks(N_(2),NO_(3)^(-),NO_(2)^(-),and NO).We also highlight the critical role of in situ and operando characterization techniques in identifying active sites and reaction intermediates,as well as progress in catalyst design.By integrating mechanistic insights,analytical advances,and materials innovation,we outline key challenges and propose actionable strategies to advance scalable and sustainable ammonia synthesis.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
High-entropy oxides(HEOs),with their multi-principal-element compositional diversity,have emerged as promising candidates in the realm of energy materials.This review encapsulates the progress in harnessing HEOs for e...High-entropy oxides(HEOs),with their multi-principal-element compositional diversity,have emerged as promising candidates in the realm of energy materials.This review encapsulates the progress in harnessing HEOs for energy conversion and storage applications,encompassing solar cells,electrocatalysis,photocatalysis,lithium-ion batteries,and solid oxide fuel cells.The critical role of theoretical calculations and simulations is underscored,highlighting their contribution to elucidating material stability,deciphering structure-activity relationships,and enabling performance optimization.These computational tools have been instrumental in multi-scale modeling,high-throughput screening,and integrating artificial intelligence for material design.Despite their promise,challenges such as fabrication complexity,cost,and theoretical computational hurdles impede the broad application of HEOs.To address these,this review delineates future research perspectives.These include the innovation of cost-effective synthesis strategies,employment of in situ characterization for micro-chemical insights,exploration of unique physical phenomena to refine performance,and enhancement of computational models for precise structure-performance predictions.This review calls for interdisciplinary synergy,fostering a collaborative approach between materials science,chemistry,physics,and related disciplines.Collectively,these efforts are poised to propel HEOs towards commercial viability in the new energy technologies,heralding innovative solutions to pressing energy and environmental challenges.展开更多
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.
基金supported by the National Natural Science Foundation of China (No.62204067)Young Talent Support Project of Guangzhou Association for Science and Technology (No.QT-2023-051)+2 种基金industry support from Shenzhen Jinjia jituan Co.,Ltd with funding No.R00043the financial support from the Science and Technology Development Fund,Macao SAR (File no.FDCT-0125/2022/A and FDCT-0006/2023/RIB1)the National Natural Science Foundation of China (No.22305009)
文摘Sustainable and clean hydrogen development has been considered a mainstream trend in contemporary energy research.Heterogenous photo(electro)catalysis is a promising approach to producing hydrogen in an environmentally friendly manner.Perovskites have emerged as an inexpensive,earth-abundant,and easily fabricated semiconductor material for photo(electro)catalysis.However,some of their shortcomings have limited the wide range of applications.In this mini-review,we present the fundamentals and applications of various perovskites for photo(electro)catalytic water splitting.In addition,we summarize advanced strategies for photo(electro)catalytic water splitting based on perovskites,focusing on the following approaches:intrinsic modulation of perovskites,functionalization of perovskites,and design of perovskite tandem systems.In summary,we point out the challenges and potential applications for perovskite solar water splitting and systematically describe various strategies to improve the photo(electro)catalysis performance of perovskites,illustrating the potential of using perovskites as key materials for solar water splitting.
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.
文摘Efficient,stable,and noble‐metal‐free electrocatalysts for both the oxygen evolution reaction and the hydrogen evolution reaction are highly imperative for the realization of low‐cost commercial water‐splitting electrolyzers.Herein,a cost‐effective and ecofriendly strategy is reported to fabricate coral‐like FeNi(OH)x/Ni as a bifunctional electrocatalyst for overall water splitting in alkaline media.With the assistance of mild corrosion of Ni by Fe(NO3)3,in situ generated FeNi(OH)x nanosheets are intimately attached on metallic coral‐like Ni.Integration of these nanosheets with the electrodeposited coral‐like Ni skeleton and the supermacroporous Ni foam substrate forms a binder‐free hierarchical electrode,which is beneficial for exposing catalytic active sites,accelerating mass transport,and facilitating the release of gaseous species.In 1.0 mol L^-1 KOH solution,a symmetric electrolyzer constructed with FeNi(OH)x/Ni as both the anode and the cathode exhibits an excellent activity with an applied potential difference of 1.52 V at 10 mA cm^-2,which is superior to that of an asymmetric electrolyzer constructed with the state‐of‐the‐art RuO2‐PtC couple(applied potential difference of 1.55 V at 10 mA cm^-2).This work contributes a facile and reliable strategy for manufacturing affordable,practical,and promising water‐splitting devices.
文摘The Ti base PbO 2 electrode prepared by electrodeposition of PbO 2 on the surface of titanium was used for electro catalytic oxidation of phenol in waste water. The experimental results show that the electrodeposition of PbO 2 at a higher current density for a short time, then followed by a lower current density can get a compact and combinative PbO 2 layer. The properties of a Ti/PbO 2 electrode with an interlayer of oxide are the best. When this kind of electrode is used to treat phenol containing waste water, the phenol removal rate is higher and the slot voltage is lower. In addition, by using the phenol removal rate as an index, the influences of electrolysis current density, mass transfer condition and pH were studied and the optimal condition was confirmed.
基金supported by the BRICS STI Framework Programme(No.52261145703)the Higher Education Discipline Innovation Project(National 111 Project,No.B16016)the Guangxi Key Research and Development Plan Project(AB24010117).
文摘Photocatalytic membranes hold significant potential for promoting pollutant degradation and reducing membrane fouling in filtration systems.Although extensive research has been conducted on the independent design of photocatalysts or membrane materials to improve their catalytic and filtration performance,the complex structures and interface mechanisms,as well as insufficient light utilization,are still often overlooked,limiting the overall performance improvement of photocatalytic membranes.This work provides an overview of enhancement strategies involving restricted area effects,external fields,such as mechanical,magnetic,thermal,and electrical fields,as well as coupling techniques with advanced oxidation processes(e.g.,O_(3),Fenton,and persulfate oxidation)for dual enhancement of photocatalysts and membranes.In addition,the synthesis method of photocatalytic membranes and the influence of factors,such as light source type,frequency,and relative position on photocatalytic membrane performance were also studied.Finally,economic feasibility and pollutant removal performance were further evaluated to determine the promising enhancement strategies,paving the way for more efficient and scalable applications of photocatalytic membranes.
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supported by the National Key Research and Development Program of China(2021YFA1500100)the National Natural Science Foundation of China(22031008)the Science Foundation of Wuhan(2020010601012192)。
文摘Reported here is a precise electro-reduction strategy for radical defluorinative alkylation towards the synthesis of gem-difluoroalkenes from α-trifluoromethylstyrenes. According to the redox-potential difference of the radical precursors, direct or indirect electrolysis is respectively adopted to realize the precise reduction. An easy-to-handle, catalyst-and metal-free condition is developed for the reduction of alkyl radical precursors that are generally easier to be reduced than α-trifluoromethylstyrenes,while a novel electro-Ni-catalytic system is established for the electro-reduction of alkyl bromides or chlorides towards the electrochemical synthesis of gem-difluoroalkenes. The merit of this protocol is exhibited by its mild conditions, wide substrate scope, and scalable preparation. Mechanistic studies and DFT calculations proved that the coordination of α-trifluoromethylstyrenes to Ni-catalyst prevents the direct reduction of the alkene and, in turn, promotes the activation of alkyl bromide through halogen atom transfer mechanism.
基金financial support from the National Natural Science Foundation of China (22373027)financial support from the Commonwealth Scientific and Industrial Research Organisation (CSIRO) Revolutionary Energy Storage Systems Future Science Platform。
文摘Ammonia is a cornerstone of global agriculture and chemical manufacturing,with emerging potential as a carbon-free energy carrier.However,its conventional production via the Haber-Bosch process is energy-intensive,relies heavily on fossil fuels,and results in significant CO_(2) emissions.In pursuit of sustainable alternatives,renewable energy-driven synthesis routes have attracted growing interest.This review surveys recent advances in green ammonia production,covering electrocatalytic,photocatalytic,photo-electrocatalytic,and photothermal pathways,with an emphasis on the mechanistic understanding of nitrogen reduction from various feedstocks(N_(2),NO_(3)^(-),NO_(2)^(-),and NO).We also highlight the critical role of in situ and operando characterization techniques in identifying active sites and reaction intermediates,as well as progress in catalyst design.By integrating mechanistic insights,analytical advances,and materials innovation,we outline key challenges and propose actionable strategies to advance scalable and sustainable ammonia synthesis.
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financial support from the Key Research and Development Program of Yunnan Province(Grant No.202302AF080002)。
文摘High-entropy oxides(HEOs),with their multi-principal-element compositional diversity,have emerged as promising candidates in the realm of energy materials.This review encapsulates the progress in harnessing HEOs for energy conversion and storage applications,encompassing solar cells,electrocatalysis,photocatalysis,lithium-ion batteries,and solid oxide fuel cells.The critical role of theoretical calculations and simulations is underscored,highlighting their contribution to elucidating material stability,deciphering structure-activity relationships,and enabling performance optimization.These computational tools have been instrumental in multi-scale modeling,high-throughput screening,and integrating artificial intelligence for material design.Despite their promise,challenges such as fabrication complexity,cost,and theoretical computational hurdles impede the broad application of HEOs.To address these,this review delineates future research perspectives.These include the innovation of cost-effective synthesis strategies,employment of in situ characterization for micro-chemical insights,exploration of unique physical phenomena to refine performance,and enhancement of computational models for precise structure-performance predictions.This review calls for interdisciplinary synergy,fostering a collaborative approach between materials science,chemistry,physics,and related disciplines.Collectively,these efforts are poised to propel HEOs towards commercial viability in the new energy technologies,heralding innovative solutions to pressing energy and environmental challenges.
