High-energy lithium-sulfur batteries(LSBs)have experienced relentless development over the past decade with discernible improvements in electrochemical performance.However,a scrutinization of the cell operation condit...High-energy lithium-sulfur batteries(LSBs)have experienced relentless development over the past decade with discernible improvements in electrochemical performance.However,a scrutinization of the cell operation conditions reveals a huge gap between the demands for practical batteries and those in the literature.Low sulfur loading,a high electrolyte/sulfur(E/S)ratio and excess anodes for lab-scale LSBs significantly offset their high-energy merit.To approach practical LSBs,high loading and lean electrolyte parameters are needed,which involve budding challenges of slow charge transfer,polysulfide precipitation and severe shuttle effects.To track these obstacles,the exploration of electrocatalysts to immobilize polysulfides and accelerate Li-S redox kinetics has been widely reported.Herein,this review aims to survey state-of-the-art catalytic materials for practical LSBs with emphasis on elucidating the correlation among catalyst design strategies,material structures and electrochemical performance.We also statistically evaluate the state-of-the-art catalyst-modified LSBs to identify the remaining discrepancy between the current advancements and the real-world requirements.In closing,we put forward our proposal for a catalytic material study to help realize practical LSBs.展开更多
Developing robust oxygen electrocatalyst with high-performance is very significant for practical rechargeable Zn-air battery.We report herein the preparation of three-dimensional continuous nanocarbon network composed...Developing robust oxygen electrocatalyst with high-performance is very significant for practical rechargeable Zn-air battery.We report herein the preparation of three-dimensional continuous nanocarbon network composed of interconnected nitrogen-doped carbon nanotubes and its application as oxygen electrocatalysis in rechargeable Zn-air battery.Except the excellent electrochemical bifunctionality,this carbon nanotube matrix also delivers an impressive battery performance.Specifically,an opencircuit voltage of 1.50 V as well as a high power density of 220 m W cm^(-2) with remarkable cycling stability for 1600 h is achieved in the rechargeable Zn-air battery.The study not only provides an efficient bifunctional oxygen electrocatalyst but more importantly may pave significant concepts in designing robust electrode for long-life rechargeable Zn-air battery and other energy technologies.展开更多
Direct methanol fuel cells are one of the most promising alternative energy technologies in the foreseeable future, but its successful commercialization in large scale is still heavily hindered by several technical sh...Direct methanol fuel cells are one of the most promising alternative energy technologies in the foreseeable future, but its successful commercialization in large scale is still heavily hindered by several technical shortfalls, especially the undesirable activity and durability issues of electrocatalysts toward methanol oxidation reaction. In light of these challenges, the inherent advantages of unsupported Pt based nanostructures demonstrate their great potentials as durable and efficient electrocatalysts for direct methanol fuel cells. This review will summarize recent achievements of unsupported Pt-based electrocatalysts toward methanol oxidation, with highlighting the interactions between the performance and structure tailoring and composition modulating. At last, a perspective is proposed for the upcoming challenges and possible opportunities to further prompt the practical application of unsupported Pt-based electrocatalysts for direct methanol fuel cells.展开更多
Oxygen electrocatalysts are of great importance for the air electrode in zinc-air batteries(ZABs).Owing to the high specific surface area,controllable pore size and unsaturated metal active sites,metal-organic framewo...Oxygen electrocatalysts are of great importance for the air electrode in zinc-air batteries(ZABs).Owing to the high specific surface area,controllable pore size and unsaturated metal active sites,metal-organic frameworks(MOFs)derivatives have been widely studied as oxygen electrocatalysts in ZABs.To date,many strategies have been developed to generate efficient oxygen electrocatalysts from MOFs for improving the performance of ZABs.In this review,the latest progress of the MOF-derived non-noble metal-oxygen electrocatalysts in ZABs is reviewed.The performance of these MOF-derived catalysts toward oxygen reduction,and oxygen evolution reactions is discussed based on the categories of metal-free carbon materials,single-atom catalysts,metal cluster/carbon composites and metal compound/carbon composites.Moreover,we provide a comprehensive overview on the design strategies of various MOF-derived non-noble metal-oxygen electrocatalysts and their structure-performance relationship.Finally,the challenges and perspectives are provided for further advancing the MOF-derived oxygen electrocatalysts in ZABs.展开更多
Electrocatalysis is essential in the conversion of chemicals to electrical energy.The search for high‐performance electrocatalysts is particularly important in the context of numerous renewable energy conversion and ...Electrocatalysis is essential in the conversion of chemicals to electrical energy.The search for high‐performance electrocatalysts is particularly important in the context of numerous renewable energy conversion and storage technologies,capable of addressing energy and environmental concerns.Electrocatalysis is used in advanced renewable energy conversion and storage technologies,such as carbon dioxide and water electrolyzers,fuel cells,metal‐air batteries,etc.For instance,the electrochemical carbon dioxide reduction(CO_(2)RR)is a green technology that can convert intermittent renewable energy sources(such as solar energy and wind energy)into fuels and valuable chemicals.Similarly,water electrocatalysis produces green and renewable fuel(hydrogen),which will not cause harm to environment.The recent decade has witnessed new ideas,materials。展开更多
丰富的中性海水有望替代高纯淡水用于绿氢制备,然而基于过渡金属材料催化的直接海水电解会因析氯反应(ClER)引发严重的腐蚀问题并造成二次重金属污染,且析氧反应(OER)的动力学缓慢.本工作中,我们报道了一种稳定的富吡啶氮的碳纸(N-CP-80...丰富的中性海水有望替代高纯淡水用于绿氢制备,然而基于过渡金属材料催化的直接海水电解会因析氯反应(ClER)引发严重的腐蚀问题并造成二次重金属污染,且析氧反应(OER)的动力学缓慢.本工作中,我们报道了一种稳定的富吡啶氮的碳纸(N-CP-800),可以有效地催化肼氧化反应(HzOR),以取代中性海水中的OER用于节能制氢.结合电化学实验、原位衰减全反射-表面增强傅里叶变换红外光谱表征和密度泛函理论计算,我们发现:相较于吡咯氮和石墨氮,zig和arm构型的吡啶氮更有利于决速步(^(*)H+N_(2)H_(1))的质子脱附,以促进肼氧化反应.因此,N-CP-800在中性介质中进行HzOR时,仅需0.78 V(相对于可逆氢电势)便可达到10 mA cm^(-2),低于其OER/ClER竞争反应.当N-CP-800与非贵金属析氢催化剂CoP耦合进行HzOR-复合海水电解时,仅需1.56 V的电压即可达到10 mA cm^(-2),并能稳定运行200 h,优于Pt/C和RuO_(2)标准电极对催化的海水电解.展开更多
Cu-based electrocatalysts with favorable facets and Cu^(+)can boost CO_(2) reduction to valuable multicarbon products.However,the inevitable Cu^(+)reduction and the phase evolution usually result in poor performance.H...Cu-based electrocatalysts with favorable facets and Cu^(+)can boost CO_(2) reduction to valuable multicarbon products.However,the inevitable Cu^(+)reduction and the phase evolution usually result in poor performance.Herein,we fabricate CuI nanodots with favorable(220)facets and a stable Cu^(+)state,accomplished by operando reconstruction of Cu(OH)_(2) under CO_(2)-and I--containing electrolytes for enhanced CO_(2)-to-C_(2)H_(4) conversion.Synchrotron X-ray absorption spectroscopy(XAS),in-situ Raman spectroscopy and thermodynamic potential analysis reveal the preferred formation of CuI.Vacuum gas electroresponse and density functional theory(DFT)calculations reveal that CO_(2)-related species induce the exposure of the(220)plane of Cu I.Moreover,the small size of nanodots enables the adequate contact with I^(-),which guarantees the rapid formation of Cu I instead of the electroreduction to Cu^(0).As a result,the resulting catalysts exhibit a high C2H4 Faradaic efficiency of 72.4%at a large current density of 800 m A cm^(-2) and robust stability for 12 h in a flow cell.Combined in-situ ATR-SEIRS spectroscopic characterizations and DFT calculations indicate that the(220)facets and stable Cu^(+) in CuI nanodots synergistically facilitate CO_(2)/*CO adsorption and*CO dimerization.展开更多
Due to the current situation of massive waste consumption and accumulation,the recycling and upgrading utilization of polymer materials is an effective technology to solve environmental pollution.In this work,the recy...Due to the current situation of massive waste consumption and accumulation,the recycling and upgrading utilization of polymer materials is an effective technology to solve environmental pollution.In this work,the recycling and upgrading methods of polymers are summarized,and the latest progress in polymer upcycling is discussed from the perspective of upgrading materials.The common polymer recovery methods,including mechanical recovery,chemical recovery,biocatalysis,and photocatalytic recovery,are discussed based on their mechanism and industrialized application.The upgrading products of polymers are divided into monomers,fuels and fine chemicals.The challenges and prospects of polymer degradation technology are discussed.展开更多
做氮的 graphene (NG ) 被一个新奇、灵巧、可伸缩的自底向上的方法成功地综合。退火的 NG (NG -- 一) 拥有的高特定的表面区域和一块层次多孔的质地，和在在碱、酸的媒介的氧减小反应的展出显著地改进的 electrocatalytic 活动。分子...做氮的 graphene (NG ) 被一个新奇、灵巧、可伸缩的自底向上的方法成功地综合。退火的 NG (NG -- 一) 拥有的高特定的表面区域和一块层次多孔的质地，和在在碱、酸的媒介的氧减小反应的展出显著地改进的 electrocatalytic 活动。分子的动态模拟显示了的 Ab initio 那快速的 H 转移和六成员的 N 结构的热力学的稳定性在 600 敮 x 从 pyrrolic 把包含 N 种类的转变提升了到展开更多
Metal-orga nic frameworks(MOFs),as an emerging family of porous inorga nic-organic crystal materials,exhibit widely applications in gas storage and separation,drug release,sensing,and catalysis,owing to easily adjusta...Metal-orga nic frameworks(MOFs),as an emerging family of porous inorga nic-organic crystal materials,exhibit widely applications in gas storage and separation,drug release,sensing,and catalysis,owing to easily adjustable pore sizes,uniformly distributed metal centers,high surface areas,and tunable functionalities.However,MOF crystal powders are usually difficult to be directly applied into specific devices because of their brittleness,insolubility and low compatibility.Therefore,to expand versatile MOF membranes with robustness and operational flexibility is urgent to satisfy practical applications.Although numerous reports have reviewed the synthesis and applications of MOF membranes,relatively few reports the electrocatalytic properties based on MOF membranes.Herein,this mini-review provides an overview of preparation of MOF membranes,including directed synthesis,secondary growth and electrochemical deposition method.Meanwhile,fabrication of ultrathin 2D MOF nanosheets those can be also defined as a kind of nanoscale MOF membranes is also mentioned.Electrocatalytic performance of oxygen reduction reaction(ORR),oxygen evolution reaction(OER),hydrogen evolution reaction(HER)and CO2 reduction reaction(CO2RR) for diverse MOF membranes/nanosheets and their derivatives are introduced.展开更多
Designing earth-abundant electrocatalysts with high performance towards water oxidation is highly decisive for the sustainable energy technologies. This study develops a facile natural corrosion approach to fabricate ...Designing earth-abundant electrocatalysts with high performance towards water oxidation is highly decisive for the sustainable energy technologies. This study develops a facile natural corrosion approach to fabricate nickel-iron hydroxides for water oxidation. The resulted electrode demonstrates an outstanding activity and stability with an overpotential of 275 mV to deliver 10 mA·cm^(−2). Experimental and theoretical results suggest the corrosion-induced formation of hydroxides and their transformation to oxyhydroxides would account for this excellent performance. This work not only provides an interesting corrosion approach for the fabrication of excellent water oxidation electrode, but also bridges traditional corrosion engineering and novel materials fabrication, which would offer some insights in the innovative principles for nanomaterials and energy technologies.展开更多
Driven by the serious ecological problems,it is urgent to explore high-efficiency sustainable energy technologies.Oxygen electrocatalysis acts as important half-reactions in the emerging electrochemical energy techniq...Driven by the serious ecological problems,it is urgent to explore high-efficiency sustainable energy technologies.Oxygen electrocatalysis acts as important half-reactions in the emerging electrochemical energy techniques including electrolysis and batteries.Gel composites exhibit the merits of rich porous,superior hydrophilic,and large specific surface area,which can significantly improve the electrolyte penetration and boost the kinetics process of oxygen electrocatalysis.In this invited contribution,the advances and challenges of a novel gel materials for oxygen electrocatalysis are summarized.Starting from the structure-activity-performance relationship of gel materials,synthetic routes of nanostructured gel materials,namely,radical polymerization,sol-gel method,hydrothermal/solvothermal reactions,and ligand-substitution method,are introduced.Afterward,the gel composites are divided into polymer-based,metal-based,and carbon-based materials in turn,and their applications in oxygen electrocatalysis are discussed respectively.At the end,the perspective and challenges for advanced gel oxygen electrocatalysts are proposed.展开更多
Hydrogen energy could be a economic and powerful technology for sustainable future. Producing hydrogen fuel by electrochemical water splitting has attracted intense interest. Due to their physical and chemical propert...Hydrogen energy could be a economic and powerful technology for sustainable future. Producing hydrogen fuel by electrochemical water splitting has attracted intense interest. Due to their physical and chemical properties, two-dimensional(2 D) nanomaterials have sparked immense interest in water electrocatalysis for hydrogen production. This review focuses on the emerging nanocatalysts in 2 D nanoarchitectures for electrocatalytic hydrogen production. The fundamentals of HER are firstly depicted, following the discussion of recent advances in typical 2 D electrocatalysts for HER. The insights into the relationship among the synthetic protocols, structure, catalytic performance and thermodynamics will be discussed in details. Finally, the outlooks regarding further development of 2 D nanocatalysts for HER are proposed.We hope this review will offer a comprehensive understanding in 2 D nanocatalysts to promote electrochemical hydrogen production.展开更多
Zinc–air batteries(ZABs)are expected to be some of the most promising power sources for wearable and portable electronic devices and have received widespread research interest.As an ion conductor connecting anodes an...Zinc–air batteries(ZABs)are expected to be some of the most promising power sources for wearable and portable electronic devices and have received widespread research interest.As an ion conductor connecting anodes and cathodes,the electrolyte is critical for the overall performance of ZABs(e.g.,energy density,rechargeability,and operating voltage).Compared with liquid electrolytes,polymer-based electrolytes have superior characteristics for ZABs,such as negligible electrolyte leakage,three-phase interface stabilization,and dendrite suppression.In this perspective,we focus on recent progress in polymer-based electrolytes for ZABs.After a brief introduction to ZABs and electrolytes,we emphasize the development of polymer-based electrolytes in terms of their intrinsic properties and interfacial chemistry.Finally,challenges and viable strategies are proposed for polymer-based electrolytes in ZABs.We hope that this work will provide useful guidance to spur the development of high-performance ZABs based on advanced polymer-based electrolytes.展开更多
Converting CO_(2) into high‐value fuels and chemicals by renewable‐electricitypowered electrochemical CO_(2) reduction reaction(CRR)is a viable approach toward carbon‐emissions‐neutral processes.Unlike the thermoc...Converting CO_(2) into high‐value fuels and chemicals by renewable‐electricitypowered electrochemical CO_(2) reduction reaction(CRR)is a viable approach toward carbon‐emissions‐neutral processes.Unlike the thermocatalytic hydrogenation of CO_(2) at the solid‐gas interface,the CRR takes place at the three‐phase gas/solid/liquid interface near the electrode surface in aqueous solution,which leads to major challenges including the limited mass diffusion of CO_(2) reactant,competitive hydrogen evolution reaction,and poor product selectivity.Here we critically examine the various methods of surface and interface engineering of the electrocatalysts to optimize the microenvironment for CRR,which can address the above issues.The effective modification strategies for the gas transport,electrolyte composition,controlling intermediate states,and catalyst engineering are discussed.The key emphasis is made on the diverse atomic‐precision modifications to increase the local CO_(2) concentration,lower the energy barriers for CO_(2) activation,decrease the H2O coverage,and stabilize intermediates to effectively control the catalytic activity and selectivity.The perspectives on the challenges and outlook for the future applications of three‐phase interface engineering for CRR and other gasinvolving electrocatalytic reactions conclude the article.展开更多
基金supported by grants from the Research Grants Council of the Hong Kong Special Administrative Region,China(Poly U25216121,Poly U15303219)the National Natural Science Foundation of China for Young Scholar(52102310)the Research Committee of the Hong Kong Polytechnic University(A-PB1 M,1-BBXK,1-CD4 M,and G-UAMV)。
文摘High-energy lithium-sulfur batteries(LSBs)have experienced relentless development over the past decade with discernible improvements in electrochemical performance.However,a scrutinization of the cell operation conditions reveals a huge gap between the demands for practical batteries and those in the literature.Low sulfur loading,a high electrolyte/sulfur(E/S)ratio and excess anodes for lab-scale LSBs significantly offset their high-energy merit.To approach practical LSBs,high loading and lean electrolyte parameters are needed,which involve budding challenges of slow charge transfer,polysulfide precipitation and severe shuttle effects.To track these obstacles,the exploration of electrocatalysts to immobilize polysulfides and accelerate Li-S redox kinetics has been widely reported.Herein,this review aims to survey state-of-the-art catalytic materials for practical LSBs with emphasis on elucidating the correlation among catalyst design strategies,material structures and electrochemical performance.We also statistically evaluate the state-of-the-art catalyst-modified LSBs to identify the remaining discrepancy between the current advancements and the real-world requirements.In closing,we put forward our proposal for a catalytic material study to help realize practical LSBs.
基金financially supported by the National Natural Science Foundation of China(21802048,21805103,21805104)the Fundamental Research Funds for the Central Universities(2018KFYXKJC044,2018KFYYXJJ121,2017KFXKJC002,2017KFYXJJ164)the National 1000 Young Talents Program of China。
文摘Developing robust oxygen electrocatalyst with high-performance is very significant for practical rechargeable Zn-air battery.We report herein the preparation of three-dimensional continuous nanocarbon network composed of interconnected nitrogen-doped carbon nanotubes and its application as oxygen electrocatalysis in rechargeable Zn-air battery.Except the excellent electrochemical bifunctionality,this carbon nanotube matrix also delivers an impressive battery performance.Specifically,an opencircuit voltage of 1.50 V as well as a high power density of 220 m W cm^(-2) with remarkable cycling stability for 1600 h is achieved in the rechargeable Zn-air battery.The study not only provides an efficient bifunctional oxygen electrocatalyst but more importantly may pave significant concepts in designing robust electrode for long-life rechargeable Zn-air battery and other energy technologies.
基金financial supported by National 1000 Young Talents Program of ChinaNation Natural Science Foundation of China(21473111)+2 种基金The Innovation Foundation of Shenzhen Government(JCYJ20160408173202143)the Joint Fund of Energy Storage of Qingdao(20160012)the Innovation Research Funds of HUST(3004013109,0118013089,and 2017KFYXJJ164)
文摘Direct methanol fuel cells are one of the most promising alternative energy technologies in the foreseeable future, but its successful commercialization in large scale is still heavily hindered by several technical shortfalls, especially the undesirable activity and durability issues of electrocatalysts toward methanol oxidation reaction. In light of these challenges, the inherent advantages of unsupported Pt based nanostructures demonstrate their great potentials as durable and efficient electrocatalysts for direct methanol fuel cells. This review will summarize recent achievements of unsupported Pt-based electrocatalysts toward methanol oxidation, with highlighting the interactions between the performance and structure tailoring and composition modulating. At last, a perspective is proposed for the upcoming challenges and possible opportunities to further prompt the practical application of unsupported Pt-based electrocatalysts for direct methanol fuel cells.
基金This work is supported by the National Natural Science Foundation of China(22075092)the Program for HUST Academic Frontier Youth Team(2018QYTD15).
文摘Oxygen electrocatalysts are of great importance for the air electrode in zinc-air batteries(ZABs).Owing to the high specific surface area,controllable pore size and unsaturated metal active sites,metal-organic frameworks(MOFs)derivatives have been widely studied as oxygen electrocatalysts in ZABs.To date,many strategies have been developed to generate efficient oxygen electrocatalysts from MOFs for improving the performance of ZABs.In this review,the latest progress of the MOF-derived non-noble metal-oxygen electrocatalysts in ZABs is reviewed.The performance of these MOF-derived catalysts toward oxygen reduction,and oxygen evolution reactions is discussed based on the categories of metal-free carbon materials,single-atom catalysts,metal cluster/carbon composites and metal compound/carbon composites.Moreover,we provide a comprehensive overview on the design strategies of various MOF-derived non-noble metal-oxygen electrocatalysts and their structure-performance relationship.Finally,the challenges and perspectives are provided for further advancing the MOF-derived oxygen electrocatalysts in ZABs.
文摘Electrocatalysis is essential in the conversion of chemicals to electrical energy.The search for high‐performance electrocatalysts is particularly important in the context of numerous renewable energy conversion and storage technologies,capable of addressing energy and environmental concerns.Electrocatalysis is used in advanced renewable energy conversion and storage technologies,such as carbon dioxide and water electrolyzers,fuel cells,metal‐air batteries,etc.For instance,the electrochemical carbon dioxide reduction(CO_(2)RR)is a green technology that can convert intermittent renewable energy sources(such as solar energy and wind energy)into fuels and valuable chemicals.Similarly,water electrocatalysis produces green and renewable fuel(hydrogen),which will not cause harm to environment.The recent decade has witnessed new ideas,materials。
基金financially supported by the National Key Research and Development Program of China(2021YFA1600800)the Program for Huazhong University of Science and Technology(HUST)Academic Frontier Youth Team+1 种基金the National Natural Science Foundation of China(22075092)the Innovation and Talent Recruitment Base of New Energy Chemistry and Device(B21003)。
文摘丰富的中性海水有望替代高纯淡水用于绿氢制备,然而基于过渡金属材料催化的直接海水电解会因析氯反应(ClER)引发严重的腐蚀问题并造成二次重金属污染,且析氧反应(OER)的动力学缓慢.本工作中,我们报道了一种稳定的富吡啶氮的碳纸(N-CP-800),可以有效地催化肼氧化反应(HzOR),以取代中性海水中的OER用于节能制氢.结合电化学实验、原位衰减全反射-表面增强傅里叶变换红外光谱表征和密度泛函理论计算,我们发现:相较于吡咯氮和石墨氮,zig和arm构型的吡啶氮更有利于决速步(^(*)H+N_(2)H_(1))的质子脱附,以促进肼氧化反应.因此,N-CP-800在中性介质中进行HzOR时,仅需0.78 V(相对于可逆氢电势)便可达到10 mA cm^(-2),低于其OER/ClER竞争反应.当N-CP-800与非贵金属析氢催化剂CoP耦合进行HzOR-复合海水电解时,仅需1.56 V的电压即可达到10 mA cm^(-2),并能稳定运行200 h,优于Pt/C和RuO_(2)标准电极对催化的海水电解.
基金financially supported by The National Key Research and Development Program of China(2021YFA1600800)the Start-up Funding of the Huazhong University of Science and Technology(HUST)+2 种基金the Program for HUST Academic Frontier Youth Teamthe National Natural Science Foundation of China(22075092)the National 1000 Young Talents Program of China and The Innovation and Talent Recruitment Base of New Energy Chemistry and Device(B21003)。
文摘Cu-based electrocatalysts with favorable facets and Cu^(+)can boost CO_(2) reduction to valuable multicarbon products.However,the inevitable Cu^(+)reduction and the phase evolution usually result in poor performance.Herein,we fabricate CuI nanodots with favorable(220)facets and a stable Cu^(+)state,accomplished by operando reconstruction of Cu(OH)_(2) under CO_(2)-and I--containing electrolytes for enhanced CO_(2)-to-C_(2)H_(4) conversion.Synchrotron X-ray absorption spectroscopy(XAS),in-situ Raman spectroscopy and thermodynamic potential analysis reveal the preferred formation of CuI.Vacuum gas electroresponse and density functional theory(DFT)calculations reveal that CO_(2)-related species induce the exposure of the(220)plane of Cu I.Moreover,the small size of nanodots enables the adequate contact with I^(-),which guarantees the rapid formation of Cu I instead of the electroreduction to Cu^(0).As a result,the resulting catalysts exhibit a high C2H4 Faradaic efficiency of 72.4%at a large current density of 800 m A cm^(-2) and robust stability for 12 h in a flow cell.Combined in-situ ATR-SEIRS spectroscopic characterizations and DFT calculations indicate that the(220)facets and stable Cu^(+) in CuI nanodots synergistically facilitate CO_(2)/*CO adsorption and*CO dimerization.
基金This work is financially supported by the National Natural Science Foundation of China(22102125)The Innovation Foundation of Key Laboratory of Green Chemical Engineering Process of Ministry of Education(GCX202108)the Scientific Research Foundation of Wuhan Institute of Technology(K2021040)are also acknowledged.
文摘Due to the current situation of massive waste consumption and accumulation,the recycling and upgrading utilization of polymer materials is an effective technology to solve environmental pollution.In this work,the recycling and upgrading methods of polymers are summarized,and the latest progress in polymer upcycling is discussed from the perspective of upgrading materials.The common polymer recovery methods,including mechanical recovery,chemical recovery,biocatalysis,and photocatalytic recovery,are discussed based on their mechanism and industrialized application.The upgrading products of polymers are divided into monomers,fuels and fine chemicals.The challenges and prospects of polymer degradation technology are discussed.
基金This work is financially supported by Shanghai Institute of Ceramics, the One Hundred Talent Plan of Chinese Academy of Sciences, National Natural Science Foundation of China （No. 21307145）, Key Project for Young Researcher of State Key Laboratory of High Performance Ceramics and Superfine Microstructure, the Youth Science and Technology Talents ＂Sail＂ Program of Shanghai Municipal Science and Technology Commission （No. 15YF1413800）, and the research grant （No. 14DZ2261200） from Shanghai government.
文摘做氮的 graphene (NG ) 被一个新奇、灵巧、可伸缩的自底向上的方法成功地综合。退火的 NG (NG -- 一) 拥有的高特定的表面区域和一块层次多孔的质地，和在在碱、酸的媒介的氧减小反应的展出显著地改进的 electrocatalytic 活动。分子的动态模拟显示了的 Ab initio 那快速的 H 转移和六成员的 N 结构的热力学的稳定性在 600 敮 x 从 pyrrolic 把包含 N 种类的转变提升了到
基金Acknowledgements We acknowledge financial support by the National Natural Science Foundation of China （Nos. 21473111 and 21376122）, Fundamental Research Funds for the Central Universities （No. GK201602002）, Innovation Foundation of Shenzhen Government （No. JCYJ20160408173202143）, the Joint Fund of Energy Storage of Qingdao （No. 20160012）, and the Fundamental Research Funds of Huazhong University of Science and Technology （Nos. 3004013109 and 0118013089）. We acknowledge the support of Analytical and Testing Center of Huazhong University of Science and Technology for SEM and XPS measurements.
基金financially supported by National Natural Science Foundation of China(Nos.21805103,21805104,21802048)Fundamental Research Funds for the Central Universities(Nos.2018KFYYXJJ121,2019KFYXJJS073)National 1000 Young Talents Program of China。
文摘Metal-orga nic frameworks(MOFs),as an emerging family of porous inorga nic-organic crystal materials,exhibit widely applications in gas storage and separation,drug release,sensing,and catalysis,owing to easily adjustable pore sizes,uniformly distributed metal centers,high surface areas,and tunable functionalities.However,MOF crystal powders are usually difficult to be directly applied into specific devices because of their brittleness,insolubility and low compatibility.Therefore,to expand versatile MOF membranes with robustness and operational flexibility is urgent to satisfy practical applications.Although numerous reports have reviewed the synthesis and applications of MOF membranes,relatively few reports the electrocatalytic properties based on MOF membranes.Herein,this mini-review provides an overview of preparation of MOF membranes,including directed synthesis,secondary growth and electrochemical deposition method.Meanwhile,fabrication of ultrathin 2D MOF nanosheets those can be also defined as a kind of nanoscale MOF membranes is also mentioned.Electrocatalytic performance of oxygen reduction reaction(ORR),oxygen evolution reaction(OER),hydrogen evolution reaction(HER)and CO2 reduction reaction(CO2RR) for diverse MOF membranes/nanosheets and their derivatives are introduced.
基金This project is funded by the Program for Associate Professor of Special Appointment （Young Eastern Scholar） at Shanghai Institutions of Higher Learning （No. QD2016013）, the Natural Science Foundation of Shanghai （No. 16ZR1423500） and the National Natural Science Foundation of China （No. 51702213）. We also acknowledge financial support by the National 1000 Young Talents Program of China, the Innovation Foundation of Shenzhen Government （No. JCYJ20160408173202143）, the Joint Fund of Energy Storage of Qingdao （No. 20160012）, the Fundamental Research Funds for the Central Universities （No. 2017KFXKJC002） and the Innovation Research Funds of HUST （No. 2017KFYXJJ164）. The Program Sponsored by Shanghai Pujiang （No. 17PJ1406900） is also acknowledged. We also acknowledge the support of the Analytical and Testing Center of Huazhong University of Science and Technology for XRD, TEM, and XPS measurements.
基金This work is financially supported by the National Natural Science Foundation of China(No.22075092)China Postdoctoral Science Foundation(No.2018M642810)the Program for HUST Academic Frontier Youth Team(No.2018QYTD15)。
文摘Designing earth-abundant electrocatalysts with high performance towards water oxidation is highly decisive for the sustainable energy technologies. This study develops a facile natural corrosion approach to fabricate nickel-iron hydroxides for water oxidation. The resulted electrode demonstrates an outstanding activity and stability with an overpotential of 275 mV to deliver 10 mA·cm^(−2). Experimental and theoretical results suggest the corrosion-induced formation of hydroxides and their transformation to oxyhydroxides would account for this excellent performance. This work not only provides an interesting corrosion approach for the fabrication of excellent water oxidation electrode, but also bridges traditional corrosion engineering and novel materials fabrication, which would offer some insights in the innovative principles for nanomaterials and energy technologies.
基金financially supported by the National Natural Science Foundation of China(No.22102125)The Scientific Research Foundation of Wuhan Institute of Technology(No.K2021040)the Innovation Foundation of Key Laboratory of Green Chemical Engineering Process of Ministry of Education(No.GCX202108)are also acknowledged.
文摘Driven by the serious ecological problems,it is urgent to explore high-efficiency sustainable energy technologies.Oxygen electrocatalysis acts as important half-reactions in the emerging electrochemical energy techniques including electrolysis and batteries.Gel composites exhibit the merits of rich porous,superior hydrophilic,and large specific surface area,which can significantly improve the electrolyte penetration and boost the kinetics process of oxygen electrocatalysis.In this invited contribution,the advances and challenges of a novel gel materials for oxygen electrocatalysis are summarized.Starting from the structure-activity-performance relationship of gel materials,synthetic routes of nanostructured gel materials,namely,radical polymerization,sol-gel method,hydrothermal/solvothermal reactions,and ligand-substitution method,are introduced.Afterward,the gel composites are divided into polymer-based,metal-based,and carbon-based materials in turn,and their applications in oxygen electrocatalysis are discussed respectively.At the end,the perspective and challenges for advanced gel oxygen electrocatalysts are proposed.
基金supported by the National Natural Science Foundation of China (Nos. 22075092, 21805103)the Program for HUST Academic Frontier Youth Team (No. 2018QYTD15)+1 种基金the Innovation and Talent Recruitment Base of New Energy Chemistry and Device (No. B21003)the National 1000 Young Talents Program of China。
文摘Hydrogen energy could be a economic and powerful technology for sustainable future. Producing hydrogen fuel by electrochemical water splitting has attracted intense interest. Due to their physical and chemical properties, two-dimensional(2 D) nanomaterials have sparked immense interest in water electrocatalysis for hydrogen production. This review focuses on the emerging nanocatalysts in 2 D nanoarchitectures for electrocatalytic hydrogen production. The fundamentals of HER are firstly depicted, following the discussion of recent advances in typical 2 D electrocatalysts for HER. The insights into the relationship among the synthetic protocols, structure, catalytic performance and thermodynamics will be discussed in details. Finally, the outlooks regarding further development of 2 D nanocatalysts for HER are proposed.We hope this review will offer a comprehensive understanding in 2 D nanocatalysts to promote electrochemical hydrogen production.
基金supported by the National Natural Science Foundation of China(22075092)the Innovation and Talent Recruitment Base of New Energy Chemistry and Device(B21003).
文摘Zinc–air batteries(ZABs)are expected to be some of the most promising power sources for wearable and portable electronic devices and have received widespread research interest.As an ion conductor connecting anodes and cathodes,the electrolyte is critical for the overall performance of ZABs(e.g.,energy density,rechargeability,and operating voltage).Compared with liquid electrolytes,polymer-based electrolytes have superior characteristics for ZABs,such as negligible electrolyte leakage,three-phase interface stabilization,and dendrite suppression.In this perspective,we focus on recent progress in polymer-based electrolytes for ZABs.After a brief introduction to ZABs and electrolytes,we emphasize the development of polymer-based electrolytes in terms of their intrinsic properties and interfacial chemistry.Finally,challenges and viable strategies are proposed for polymer-based electrolytes in ZABs.We hope that this work will provide useful guidance to spur the development of high-performance ZABs based on advanced polymer-based electrolytes.
基金Australian Research Council,Grant/Award Numbers:FL170100154,FT200100062,DP220102596,DP210100472,DP190103472。
文摘Converting CO_(2) into high‐value fuels and chemicals by renewable‐electricitypowered electrochemical CO_(2) reduction reaction(CRR)is a viable approach toward carbon‐emissions‐neutral processes.Unlike the thermocatalytic hydrogenation of CO_(2) at the solid‐gas interface,the CRR takes place at the three‐phase gas/solid/liquid interface near the electrode surface in aqueous solution,which leads to major challenges including the limited mass diffusion of CO_(2) reactant,competitive hydrogen evolution reaction,and poor product selectivity.Here we critically examine the various methods of surface and interface engineering of the electrocatalysts to optimize the microenvironment for CRR,which can address the above issues.The effective modification strategies for the gas transport,electrolyte composition,controlling intermediate states,and catalyst engineering are discussed.The key emphasis is made on the diverse atomic‐precision modifications to increase the local CO_(2) concentration,lower the energy barriers for CO_(2) activation,decrease the H2O coverage,and stabilize intermediates to effectively control the catalytic activity and selectivity.The perspectives on the challenges and outlook for the future applications of three‐phase interface engineering for CRR and other gasinvolving electrocatalytic reactions conclude the article.
