The ammonia synthesis from nitrogen and water under ambient conditions is one of the most inviting but challenging reaction routes.Although nitrogen is abundant in the atmosphere and the ammonia synthesis reaction is ...The ammonia synthesis from nitrogen and water under ambient conditions is one of the most inviting but challenging reaction routes.Although nitrogen is abundant in the atmosphere and the ammonia synthesis reaction is exothermic on the thermodynamics,the conversion of N2 to ammonia is actually hard to proceed owing to the chemical inertness and stability of N2 molecules.In industry,ammonia synthesis is carried out by the Haber-Bosch process under harsh conditions (300-500 ℃,20-30 MPa) associated with the requirement of substantial energy input and the enormous emission of greenhouse gases (e.g.,CO2).Recently,a growing number of studies on photo(electro)catalytic and electrocatalytic nitrogen reduction reaction (NRR) in aqueous solution have attracted extensive attention,which holds great promise for nitrogen fixation under room temperature and atmospheric pressure.However,the very low efficiency and ambiguous mechanism still remain as the major hurdles for the development of photochemical and electrochemical NRR systems.Here we provide an overview of the latest progresses,remaining challenges and future prospects in photocatalytic and electrocatalytic nitrogen fixation.Moreover,this review offers a helpful guidance for the reasonable design of photocatalysts and electrocatalysts towards NRR by combining theory predictions and experiment results.We hope this review can stimulate more research interests in the relatively understudied but highly promising research field of NRR.展开更多
Electrocatalytic carbon dioxide(CO2)reduction(ECR)has become one of the main methods to close the broken carbon cycle and temporarily store renewable energy,but there are still some problems such as poor stability,low...Electrocatalytic carbon dioxide(CO2)reduction(ECR)has become one of the main methods to close the broken carbon cycle and temporarily store renewable energy,but there are still some problems such as poor stability,low activity,and selectivity.While the most promising strategy to improve ECR activity is to develop electrocatalysts with low cost,high activity,and long-term stability.Recently,defective carbon-based nanomaterials have attracted extensive attention due to the unbalanced electron distribution and electronic structural distortion caused by the defects on the carbon materials.Here,the present review mainly summarizes the latest research progress of the construction of the diverse types of defects(intrinsic carbon defects,heteroatom doping defects,metal atomic sites,and edges detects)for carbon materials in ECR,and unveil the structure-activity relationship and its catalytic mechanism.The current challenges and opportunities faced by high-performance carbon materials in ECR are discussed,as well as possible future solutions.It can be believed that this review can provide some inspiration for the future of development of high-performance ECR catalysts.展开更多
基金the National Key R&D Program of China (Nos.2017YFA0208200,2016YFB0700600,and 2015CB659300)the National Natural Science Foundation of China (NSFC)(Nos. 21872069,51761135104,and 21573108)+2 种基金the Natural Science Foundation of Jiangsu Province (Nos.BK20180008 and BK20150571)High-Level Entrepreneurial and Innovative Talents Program of Jiangsu Provincethe Fundamental Research Funds for the Central Universities of China (No.020514380146).
文摘The ammonia synthesis from nitrogen and water under ambient conditions is one of the most inviting but challenging reaction routes.Although nitrogen is abundant in the atmosphere and the ammonia synthesis reaction is exothermic on the thermodynamics,the conversion of N2 to ammonia is actually hard to proceed owing to the chemical inertness and stability of N2 molecules.In industry,ammonia synthesis is carried out by the Haber-Bosch process under harsh conditions (300-500 ℃,20-30 MPa) associated with the requirement of substantial energy input and the enormous emission of greenhouse gases (e.g.,CO2).Recently,a growing number of studies on photo(electro)catalytic and electrocatalytic nitrogen reduction reaction (NRR) in aqueous solution have attracted extensive attention,which holds great promise for nitrogen fixation under room temperature and atmospheric pressure.However,the very low efficiency and ambiguous mechanism still remain as the major hurdles for the development of photochemical and electrochemical NRR systems.Here we provide an overview of the latest progresses,remaining challenges and future prospects in photocatalytic and electrocatalytic nitrogen fixation.Moreover,this review offers a helpful guidance for the reasonable design of photocatalysts and electrocatalysts towards NRR by combining theory predictions and experiment results.We hope this review can stimulate more research interests in the relatively understudied but highly promising research field of NRR.
基金the National Natural Science Foundation of China(No.21875221,21571157,U1604123,and 21773016)the Youth Talent Support Program of High-Level Talents Special Support Plan in Henan Province(ZYQR201810148)+1 种基金Creative talents in the Education Department of Henan Province(19HASTIT039)the project supported by State Key Laboratory of Advanced Technology for Materials Synthesis and Processing(Wuhan University of Technology)(2019-KF-13).
文摘Electrocatalytic carbon dioxide(CO2)reduction(ECR)has become one of the main methods to close the broken carbon cycle and temporarily store renewable energy,but there are still some problems such as poor stability,low activity,and selectivity.While the most promising strategy to improve ECR activity is to develop electrocatalysts with low cost,high activity,and long-term stability.Recently,defective carbon-based nanomaterials have attracted extensive attention due to the unbalanced electron distribution and electronic structural distortion caused by the defects on the carbon materials.Here,the present review mainly summarizes the latest research progress of the construction of the diverse types of defects(intrinsic carbon defects,heteroatom doping defects,metal atomic sites,and edges detects)for carbon materials in ECR,and unveil the structure-activity relationship and its catalytic mechanism.The current challenges and opportunities faced by high-performance carbon materials in ECR are discussed,as well as possible future solutions.It can be believed that this review can provide some inspiration for the future of development of high-performance ECR catalysts.
