Water splitting powered by clean electricity is a sustainable and promising approach to produce green hydrogen.Currently,noble metal(e.g.Iridium,Ruthenium,Platinum)-based catalysts are most widely used for water split...Water splitting powered by clean electricity is a sustainable and promising approach to produce green hydrogen.Currently,noble metal(e.g.Iridium,Ruthenium,Platinum)-based catalysts are most widely used for water splitting electrolysis.However,noble metal-based catalysts often suffer from multiple disadvantages,including high cost,low selectivity and poor durability.The emergence of metal-organic framework nanosheets(MOFNSs)attracts significant attention due to their unique advantages.Here,a concise,yet comprehensive and critical,review of recent advances in the field of MOFNSs is provided.This review explains the fundamental oxygen evolution reaction(OER)and hydrogen evolution reaction(HER)catalytic mechanisms as well as key characterization techniques for the structure-activity relationship study are discussed.Moreover,it discusses efficient design strategies and the brief research advances of MOFNSs in HER,OER,and bifunctional electrocatalysis,along with some challenges and opportunities.展开更多
A novel marine microbial esterase PHE14 was cloned from the genome of Pseudomonas oryzihabit‐ans HUP022 isolated from the deep sea of the western Pacific Ocean. Esterase PHE14 exhibited very good tolerance to most or...A novel marine microbial esterase PHE14 was cloned from the genome of Pseudomonas oryzihabit‐ans HUP022 isolated from the deep sea of the western Pacific Ocean. Esterase PHE14 exhibited very good tolerance to most organic solvents, surfactants and metal ions tested, thus making it a good esterase candidate for organic synthesis that requires an organic solvent, surfactants or metal ions. Esterase PHE14 was utilized as a biocatalyst in the asymmetric synthesis of D‐methyl lactate by enzymatic kinetic resolution. D‐methyl lactate is a key chiral chemical. Contrary to some previous reports, the addition of an organic solvent and surfactants in the enzymatic reaction did not have a beneficial effect on the kinetic resolution catalyzed by esterase PHE14. Our study is the first report on the preparation of the enantiomerically enriched product D‐methyl lactate by enzymatic kinetic resolution. The desired enantiomerically enriched product D‐methyl lactate was obtained with a high enantiomeric excess of 99%and yield of 88.7%after process optimization. The deep sea mi‐crobial esterase PHE14 is a green biocatalyst with very good potential in asymmetric synthesis in industry and can replace the traditional organic synthesis that causes pollution to the environment.展开更多
Developing highly active catalysts for photo/electrocatalytic water splitting is an attractive strategy to produce H2 as a renewable energy source.In this study,a new nickel boron oxide/graphdiyne(NiBi/GDY)hybrid cata...Developing highly active catalysts for photo/electrocatalytic water splitting is an attractive strategy to produce H2 as a renewable energy source.In this study,a new nickel boron oxide/graphdiyne(NiBi/GDY)hybrid catalyst was prepared by a facile synthetic approach.Benefitting from the strong electron donating ability of graphdiyne,NiBi/GDY showed an optimized electronic structure containing lower valence nickel atoms and demonstrated improved catalytic performance.As expected,NiBi/GDY displayed a high photocatalytic H2 evolution rate of 4.54 mmol g^(-1)h^(-1),2.9 and 4.5 times higher than those of NiBi/graphene and NiBi,respectively.NiBi/GDY also displayed outstanding electrocatalytic H2 evolution activity in 1.0 M KOH solution,with a current density of 400 mA/cm^(2)at an overpotential of 478.0 mV,which is lower than that of commercial Pt/C(505.3 mV@400 mA/cm^(2)).This work demonstrates that GDY is an ideal support for the development of highly active catalysts for photo/electrocatalytic H2 evolution.展开更多
Electrochemical water splitting consists of two elementary reactions i.e.,hydrogen evolution reaction(HER)and oxygen evolution reaction(OER).Developing robust HER and OER technologies necessitates a molecular picture ...Electrochemical water splitting consists of two elementary reactions i.e.,hydrogen evolution reaction(HER)and oxygen evolution reaction(OER).Developing robust HER and OER technologies necessitates a molecular picture of reaction mechanism,yet the reactants for water splitting reactions are unfortunately not fully understood.Here we utilize magnetic field to understand proton transport in HER,and hydroxide ion transport in OER,to discuss the possible implications on understanding the reactants for HER and OER.Magnetic field is a known tool for changing the movement of charged species like ions,e.g.the magnetic‐field‐improved Cu^(2+)transportation near the electrode in Cu electrodeposition.However,applying a magnetic field does not affect the HER or OER rate across various pH,which challenges the traditional opinion that charged species(i.e.proton and hydroxide ion)act as the reactant.This anomalous response of HER and OER to magnetic field,and the fact that the transport of proton and hydroxide ion follow Grotthuss mechanism,collectively indicate water may act as the universal reactant for HER and OER across various pH.With the aid of magnetic field,this work serves as an understanding of water might be the reactant in HER and OER,and possibly in other electrocatalysis reactions involving protonation and deprotonation step.A model that simply focuses on the charged species but overlooking the complexity of the whole electrolyte phase where water is the dominant species,may not reasonably reflect the electrochemistry of HER and OER in aqueous electrolyte.展开更多
The kinetics of non-catalyzed decompositions of xylose and its decomposition product furfural in high temperature liquid water (HTLW) was studied for temperature from 180 to 220℃ and under pressure of 10MPa. The ma...The kinetics of non-catalyzed decompositions of xylose and its decomposition product furfural in high temperature liquid water (HTLW) was studied for temperature from 180 to 220℃ and under pressure of 10MPa. The main products of xylose decomposition were furfural and formic acid, and furfural further degraded to formic acid under HTLW condition. With the assumption of first order kinetics e.quation, the evaluated activation energy of xylose and furfural decomposition was 123.27kJ·mol^-1 and 58.84kJ·mol^-1, respectively.展开更多
Two-dimensional carbides,nitrides,and carbonitrides(MXenes)play important roles in promoting the development of sustainable energy because they have abundant reactive sites on their surfaces.An increasing number of MX...Two-dimensional carbides,nitrides,and carbonitrides(MXenes)play important roles in promoting the development of sustainable energy because they have abundant reactive sites on their surfaces.An increasing number of MXenes with diverse elements and composites have been predicted and synthesized for electrocatalysis applications since the first report of a Ti-Mo-based MXene for the hydrogen evolution reaction(HER).Herein,we summarize the progress of MXene-based electrocatalysts for the HER,the oxygen evolution reaction,and the oxygen reduction reaction,including regulated pristine MXenes and modified hybrid MXenes,from both theoretical and experimental perspectives.A brief overview on MXene synthesis is presented first,accompanied by a discussion on the relationship between electrocatalytic properties and M,X,T,vacancies,and morphologies.After reviewing strategies in terms of atom substitution,functional modification,defect engineering,and morphology control,we emphasize the construction of heterojunctions between MXenes and other nanostructures,such as metal nanoparticles,oxides,hydroxides,sulfides,and phosphides.We finally discuss prospects for the future development of MXene-based electrocatalysts.展开更多
Hydrogen is a promising sustainable energy to replace fossil fuels owning to its high specific energy and environmental friendliness.Alkaline water electrolysis has been considered as one of the most prospective techn...Hydrogen is a promising sustainable energy to replace fossil fuels owning to its high specific energy and environmental friendliness.Alkaline water electrolysis has been considered as one of the most prospective technologies for large scale hydrogen production.To boost the sluggish kinetics of hydrogen evolution reaction(HER)in alkaline media,abundant materials have been designed and fabricated.Herein,we summarize the key achievements in the development of layered transition-metal hydroxides[TM(OH)x]for efficient alkaline HER.Based on the structure of TM(OH)x,the mechanism of synergistic effect between TM(OH)x and HER active materials is illuminated firstly.Then,recent progress of TM(OH)x-based HER catalysts to optimize the synergistic effect are categorized as TM(OH)x and active materials,including species,structure,morphology and interaction relationship.Furthermore,TM(OH)x-based overall water splitting electrocatalysts and electrodes are summarized in the design principles for high activity and stability.Finally,some of key challenges for further developments and applications of hydrogen production are proposed.展开更多
Cation substitution in spinel cobaltites(e.g.,ACo2O4,in which A=Mn,Fe,Co,Ni,Cu,or Zn)is a promising strategy to precisely modulate their electronic structure/properties and thus improve the corresponding electrochemic...Cation substitution in spinel cobaltites(e.g.,ACo2O4,in which A=Mn,Fe,Co,Ni,Cu,or Zn)is a promising strategy to precisely modulate their electronic structure/properties and thus improve the corresponding electrochemical performance for water splitting.However,the fundamental principles and mechanisms are not fully understood.This research aims to systematically investigate the effects of cation substitution in spinel cobaltites derived from mixed-metal-organic frameworks on the oxygen evolution reaction(OER).Among the obtained ACo2O4 catalysts,FeCo2O4 showed excellent OER performance with a current density of 10 mA·cm^-2 at an overpotential of 164 mV in alkaline media.Both theoretical calculations and experimental results demonstrate that the Fe substitution in the crystal lattice of ACo2O4 can significantly accelerate charge transfer,thereby achieving enhanced electrochemical properties.The crystal field of spinel ACo2O4,which determines the valence states of cations A,is identified as the key factor to dictate the OER performance of these spinel cobaltites.展开更多
Photocatalytic Z-scheme water splitting is considered as a promising approach to produce solar hydrogen.However,the forward hydrogen production reaction is often impeded by backward reactions.In the present study,in a...Photocatalytic Z-scheme water splitting is considered as a promising approach to produce solar hydrogen.However,the forward hydrogen production reaction is often impeded by backward reactions.In the present study,in a photosystem Ⅱ-integrated hybrid Z-scheme water splitting system,the backward hydrogen oxidation reaction was significantly suppressed by loading a PtCrOx cocatalyst on a ZrO2/TaON photocatalyst.Due to the weak chemisorption and activation of molecular hydrogen on PtCrOx,where Pt is stabilized in the oxidized forms,Pt^Ⅱ and Pt^Ⅳ,hydrogen oxidation is inhibited.However,it is remarkably well-catalyzed by the metallic Pt cocatalyst,thereby rapidly consuming the produced hydrogen.This work describes an approach to inhibit the backward reaction in the photosystem Ⅱ-integrated hybrid Z-scheme water splitting system using Fe(CN)6^3-/Fe(CN)6^4-redox couple as an electron shuttle.展开更多
Alkaline water splitting is a promising technology for“green hydrogen”generation.To improve its efficiency,highly robust catalysts are required to reduce the overpotential for low electrical power consumption.Hetero...Alkaline water splitting is a promising technology for“green hydrogen”generation.To improve its efficiency,highly robust catalysts are required to reduce the overpotential for low electrical power consumption.Heteroatom modification is one of the most effective strategies for boosting catalytic performance,as it can regulate the physicochemical properties of host catalysts to improve their intrinsic activity.Herein,aiming to provide an overview of the impact of heteroatoms on catalytic activity at the atomic level,we present a review of the key role of heteroatoms in enhancing reaction kinetics based on the reaction pathways of the hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)in alkaline media.In particular,the introduction of heteroatoms can directly and indirectly optimize the interactions between the active sites and intermediates,thus improving the intrinsic activity.To clearly illustrate this influence in detail,we have summarized a series of representative heteroatom-modified electrocatalysts and discussed the important roles of heteroatoms in the OER and HER reaction pathways.Finally,some challenges and perspectives for heteroatom-modified electrodes are discussed.We hope that this review will be helpful for the development of efficient and low-cost electrocatalysts for water electrolysis and other energy conversion applications.展开更多
Nano‐catalysis plays a vital role in the chemical transformations and significantly impacts the booming modern chemical industry.The rapid technological enhancements have resulted in serious energy and environmental ...Nano‐catalysis plays a vital role in the chemical transformations and significantly impacts the booming modern chemical industry.The rapid technological enhancements have resulted in serious energy and environmental issues,which are currently spurring the exploration of the novel nano‐catalysts in diverse fields.In order to develop the efficient nano‐catalysts,it is essential to understand their fundamental physicochemical properties,including the coordination structures of the active centers and substrate‐adsorbate interactions.Subsequently,the nano‐catalyst design with precise manipulation at the atomic level can be attained.In this account,we have summarized our extensive investigation of the factors impacting nano‐catalysis,along with the synthetic strategies developed to prepare the nano‐catalysts for applications in electrocatalysis,photocatalysis and thermocatalysis.Finally,a brief conclusion and future research directions on nano‐catalysis have also been presented.展开更多
Catalytic water splitting potentially reduce the consumption of fossil fuels and has received intense research attention.Synergy effects in multi‐element transition metal‐based water splitting catalysts have evoked ...Catalytic water splitting potentially reduce the consumption of fossil fuels and has received intense research attention.Synergy effects in multi‐element transition metal‐based water splitting catalysts have evoked special interests.Studies on catalysts in interfacial structures are especially meaningful due to their pertinence in applications.In this study,we report the synergy effects in promoting catalytic power in the ternary transition metal Zn,Co,Ni alloy nanoparticles that embeds in the carbonized Ppy/CNT multilayered matrix.By comparison with a series of binary or single metal counterparts,the mechanism under the synergy effects are elucidated.Experimental and DFT calculation results indicate that the ternary transition metal catalysts in the N‐doped carbon matrix present special electronic structure,which benefits the reversible transition‐state adsorption in HER and OER and render the catalysts high conductivity in room temperature.We expect our findings inspire further development of efficient transition metal HER and OER catalysts.展开更多
The influences of kinds and level of catalyst, time of decomposition reaction on the distribution of dibasic acid and apparent yield of adipic acid were researched; the acidic washing waste water (BI waste water) pr...The influences of kinds and level of catalyst, time of decomposition reaction on the distribution of dibasic acid and apparent yield of adipic acid were researched; the acidic washing waste water (BI waste water) producing from the equipment of cyclohexane oxidation by air was as stuff, the component of products by decomposed and oxidated in different conditions were analysed. It indicated that in the presence of cobalt salt the apparent yield of adipic acid was upto 10%-12% for the total BI waste water after the concentrated BI waste water refluxed for two hours, and then oxidated by nitric acid.展开更多
基金supported by the National Natural Science Foundation of China(No.21972124,No.21603041)the Priority Academic Program Development of Jiangsu Higher Education Institution。
文摘Water splitting powered by clean electricity is a sustainable and promising approach to produce green hydrogen.Currently,noble metal(e.g.Iridium,Ruthenium,Platinum)-based catalysts are most widely used for water splitting electrolysis.However,noble metal-based catalysts often suffer from multiple disadvantages,including high cost,low selectivity and poor durability.The emergence of metal-organic framework nanosheets(MOFNSs)attracts significant attention due to their unique advantages.Here,a concise,yet comprehensive and critical,review of recent advances in the field of MOFNSs is provided.This review explains the fundamental oxygen evolution reaction(OER)and hydrogen evolution reaction(HER)catalytic mechanisms as well as key characterization techniques for the structure-activity relationship study are discussed.Moreover,it discusses efficient design strategies and the brief research advances of MOFNSs in HER,OER,and bifunctional electrocatalysis,along with some challenges and opportunities.
基金supported by the Strategic Priority Research Program of the Chinese Academy of Sciences (XDA11030404)Key Project from the Chinese Academy of Sciences (KGZD-EW-606)+1 种基金the National Natural Science Foundation of China (21302199)Guangzhou Science and Technology Plan Projects (201510010012)~~
文摘A novel marine microbial esterase PHE14 was cloned from the genome of Pseudomonas oryzihabit‐ans HUP022 isolated from the deep sea of the western Pacific Ocean. Esterase PHE14 exhibited very good tolerance to most organic solvents, surfactants and metal ions tested, thus making it a good esterase candidate for organic synthesis that requires an organic solvent, surfactants or metal ions. Esterase PHE14 was utilized as a biocatalyst in the asymmetric synthesis of D‐methyl lactate by enzymatic kinetic resolution. D‐methyl lactate is a key chiral chemical. Contrary to some previous reports, the addition of an organic solvent and surfactants in the enzymatic reaction did not have a beneficial effect on the kinetic resolution catalyzed by esterase PHE14. Our study is the first report on the preparation of the enantiomerically enriched product D‐methyl lactate by enzymatic kinetic resolution. The desired enantiomerically enriched product D‐methyl lactate was obtained with a high enantiomeric excess of 99%and yield of 88.7%after process optimization. The deep sea mi‐crobial esterase PHE14 is a green biocatalyst with very good potential in asymmetric synthesis in industry and can replace the traditional organic synthesis that causes pollution to the environment.
文摘Developing highly active catalysts for photo/electrocatalytic water splitting is an attractive strategy to produce H2 as a renewable energy source.In this study,a new nickel boron oxide/graphdiyne(NiBi/GDY)hybrid catalyst was prepared by a facile synthetic approach.Benefitting from the strong electron donating ability of graphdiyne,NiBi/GDY showed an optimized electronic structure containing lower valence nickel atoms and demonstrated improved catalytic performance.As expected,NiBi/GDY displayed a high photocatalytic H2 evolution rate of 4.54 mmol g^(-1)h^(-1),2.9 and 4.5 times higher than those of NiBi/graphene and NiBi,respectively.NiBi/GDY also displayed outstanding electrocatalytic H2 evolution activity in 1.0 M KOH solution,with a current density of 400 mA/cm^(2)at an overpotential of 478.0 mV,which is lower than that of commercial Pt/C(505.3 mV@400 mA/cm^(2)).This work demonstrates that GDY is an ideal support for the development of highly active catalysts for photo/electrocatalytic H2 evolution.
基金supported by the Singapore MOE Tier 2 MOE2018-T2-2-027the Singapore National Research Foundation under its Campus for Research Excellence and Technological Enterprise (CREATE) Programme
文摘Electrochemical water splitting consists of two elementary reactions i.e.,hydrogen evolution reaction(HER)and oxygen evolution reaction(OER).Developing robust HER and OER technologies necessitates a molecular picture of reaction mechanism,yet the reactants for water splitting reactions are unfortunately not fully understood.Here we utilize magnetic field to understand proton transport in HER,and hydroxide ion transport in OER,to discuss the possible implications on understanding the reactants for HER and OER.Magnetic field is a known tool for changing the movement of charged species like ions,e.g.the magnetic‐field‐improved Cu^(2+)transportation near the electrode in Cu electrodeposition.However,applying a magnetic field does not affect the HER or OER rate across various pH,which challenges the traditional opinion that charged species(i.e.proton and hydroxide ion)act as the reactant.This anomalous response of HER and OER to magnetic field,and the fact that the transport of proton and hydroxide ion follow Grotthuss mechanism,collectively indicate water may act as the universal reactant for HER and OER across various pH.With the aid of magnetic field,this work serves as an understanding of water might be the reactant in HER and OER,and possibly in other electrocatalysis reactions involving protonation and deprotonation step.A model that simply focuses on the charged species but overlooking the complexity of the whole electrolyte phase where water is the dominant species,may not reasonably reflect the electrochemistry of HER and OER in aqueous electrolyte.
基金Supported by the National Natural Science Foundation of China (No.20476089) and the Project of the Ministry of Science and Technology of China (No.2004CCA05500).
文摘The kinetics of non-catalyzed decompositions of xylose and its decomposition product furfural in high temperature liquid water (HTLW) was studied for temperature from 180 to 220℃ and under pressure of 10MPa. The main products of xylose decomposition were furfural and formic acid, and furfural further degraded to formic acid under HTLW condition. With the assumption of first order kinetics e.quation, the evaluated activation energy of xylose and furfural decomposition was 123.27kJ·mol^-1 and 58.84kJ·mol^-1, respectively.
文摘Two-dimensional carbides,nitrides,and carbonitrides(MXenes)play important roles in promoting the development of sustainable energy because they have abundant reactive sites on their surfaces.An increasing number of MXenes with diverse elements and composites have been predicted and synthesized for electrocatalysis applications since the first report of a Ti-Mo-based MXene for the hydrogen evolution reaction(HER).Herein,we summarize the progress of MXene-based electrocatalysts for the HER,the oxygen evolution reaction,and the oxygen reduction reaction,including regulated pristine MXenes and modified hybrid MXenes,from both theoretical and experimental perspectives.A brief overview on MXene synthesis is presented first,accompanied by a discussion on the relationship between electrocatalytic properties and M,X,T,vacancies,and morphologies.After reviewing strategies in terms of atom substitution,functional modification,defect engineering,and morphology control,we emphasize the construction of heterojunctions between MXenes and other nanostructures,such as metal nanoparticles,oxides,hydroxides,sulfides,and phosphides.We finally discuss prospects for the future development of MXene-based electrocatalysts.
基金supported by the National Key Research and Development Program(2017YFC0306403)the Strategic Priority Research Program of the Chinese Academy of Sciences(XDA09030104,XDA22010601)the Youth Innovation Promotion Association of the Chinese Academy of Sciences~~
文摘Hydrogen is a promising sustainable energy to replace fossil fuels owning to its high specific energy and environmental friendliness.Alkaline water electrolysis has been considered as one of the most prospective technologies for large scale hydrogen production.To boost the sluggish kinetics of hydrogen evolution reaction(HER)in alkaline media,abundant materials have been designed and fabricated.Herein,we summarize the key achievements in the development of layered transition-metal hydroxides[TM(OH)x]for efficient alkaline HER.Based on the structure of TM(OH)x,the mechanism of synergistic effect between TM(OH)x and HER active materials is illuminated firstly.Then,recent progress of TM(OH)x-based HER catalysts to optimize the synergistic effect are categorized as TM(OH)x and active materials,including species,structure,morphology and interaction relationship.Furthermore,TM(OH)x-based overall water splitting electrocatalysts and electrodes are summarized in the design principles for high activity and stability.Finally,some of key challenges for further developments and applications of hydrogen production are proposed.
文摘Cation substitution in spinel cobaltites(e.g.,ACo2O4,in which A=Mn,Fe,Co,Ni,Cu,or Zn)is a promising strategy to precisely modulate their electronic structure/properties and thus improve the corresponding electrochemical performance for water splitting.However,the fundamental principles and mechanisms are not fully understood.This research aims to systematically investigate the effects of cation substitution in spinel cobaltites derived from mixed-metal-organic frameworks on the oxygen evolution reaction(OER).Among the obtained ACo2O4 catalysts,FeCo2O4 showed excellent OER performance with a current density of 10 mA·cm^-2 at an overpotential of 164 mV in alkaline media.Both theoretical calculations and experimental results demonstrate that the Fe substitution in the crystal lattice of ACo2O4 can significantly accelerate charge transfer,thereby achieving enhanced electrochemical properties.The crystal field of spinel ACo2O4,which determines the valence states of cations A,is identified as the key factor to dictate the OER performance of these spinel cobaltites.
基金supported by the Strategic Priority Research Program of Chinese Academy of Sciences(XDB17000000)the Key Research Program of Frontier Sciences,CAS(QYZDY-SSW-JSC023)+1 种基金the National Natural Science Foundation of China(21603224,31470339)the National Key R&D Program of China(2017YFA0503700)~~
文摘Photocatalytic Z-scheme water splitting is considered as a promising approach to produce solar hydrogen.However,the forward hydrogen production reaction is often impeded by backward reactions.In the present study,in a photosystem Ⅱ-integrated hybrid Z-scheme water splitting system,the backward hydrogen oxidation reaction was significantly suppressed by loading a PtCrOx cocatalyst on a ZrO2/TaON photocatalyst.Due to the weak chemisorption and activation of molecular hydrogen on PtCrOx,where Pt is stabilized in the oxidized forms,Pt^Ⅱ and Pt^Ⅳ,hydrogen oxidation is inhibited.However,it is remarkably well-catalyzed by the metallic Pt cocatalyst,thereby rapidly consuming the produced hydrogen.This work describes an approach to inhibit the backward reaction in the photosystem Ⅱ-integrated hybrid Z-scheme water splitting system using Fe(CN)6^3-/Fe(CN)6^4-redox couple as an electron shuttle.
文摘Alkaline water splitting is a promising technology for“green hydrogen”generation.To improve its efficiency,highly robust catalysts are required to reduce the overpotential for low electrical power consumption.Heteroatom modification is one of the most effective strategies for boosting catalytic performance,as it can regulate the physicochemical properties of host catalysts to improve their intrinsic activity.Herein,aiming to provide an overview of the impact of heteroatoms on catalytic activity at the atomic level,we present a review of the key role of heteroatoms in enhancing reaction kinetics based on the reaction pathways of the hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)in alkaline media.In particular,the introduction of heteroatoms can directly and indirectly optimize the interactions between the active sites and intermediates,thus improving the intrinsic activity.To clearly illustrate this influence in detail,we have summarized a series of representative heteroatom-modified electrocatalysts and discussed the important roles of heteroatoms in the OER and HER reaction pathways.Finally,some challenges and perspectives for heteroatom-modified electrodes are discussed.We hope that this review will be helpful for the development of efficient and low-cost electrocatalysts for water electrolysis and other energy conversion applications.
文摘Nano‐catalysis plays a vital role in the chemical transformations and significantly impacts the booming modern chemical industry.The rapid technological enhancements have resulted in serious energy and environmental issues,which are currently spurring the exploration of the novel nano‐catalysts in diverse fields.In order to develop the efficient nano‐catalysts,it is essential to understand their fundamental physicochemical properties,including the coordination structures of the active centers and substrate‐adsorbate interactions.Subsequently,the nano‐catalyst design with precise manipulation at the atomic level can be attained.In this account,we have summarized our extensive investigation of the factors impacting nano‐catalysis,along with the synthetic strategies developed to prepare the nano‐catalysts for applications in electrocatalysis,photocatalysis and thermocatalysis.Finally,a brief conclusion and future research directions on nano‐catalysis have also been presented.
文摘Catalytic water splitting potentially reduce the consumption of fossil fuels and has received intense research attention.Synergy effects in multi‐element transition metal‐based water splitting catalysts have evoked special interests.Studies on catalysts in interfacial structures are especially meaningful due to their pertinence in applications.In this study,we report the synergy effects in promoting catalytic power in the ternary transition metal Zn,Co,Ni alloy nanoparticles that embeds in the carbonized Ppy/CNT multilayered matrix.By comparison with a series of binary or single metal counterparts,the mechanism under the synergy effects are elucidated.Experimental and DFT calculation results indicate that the ternary transition metal catalysts in the N‐doped carbon matrix present special electronic structure,which benefits the reversible transition‐state adsorption in HER and OER and render the catalysts high conductivity in room temperature.We expect our findings inspire further development of efficient transition metal HER and OER catalysts.
文摘The influences of kinds and level of catalyst, time of decomposition reaction on the distribution of dibasic acid and apparent yield of adipic acid were researched; the acidic washing waste water (BI waste water) producing from the equipment of cyclohexane oxidation by air was as stuff, the component of products by decomposed and oxidated in different conditions were analysed. It indicated that in the presence of cobalt salt the apparent yield of adipic acid was upto 10%-12% for the total BI waste water after the concentrated BI waste water refluxed for two hours, and then oxidated by nitric acid.