We propose a facile facet regulation enabled by nanoarray architecture to achieve a high faradic efficiency of Fe_(2)O_(3) catalyst for NRR. The a-Fe_(2)O_(3) nanorod arrays (NAs) were directly grown on carbon cloth (...We propose a facile facet regulation enabled by nanoarray architecture to achieve a high faradic efficiency of Fe_(2)O_(3) catalyst for NRR. The a-Fe_(2)O_(3) nanorod arrays (NAs) were directly grown on carbon cloth (CC) with specific (104) facet exposure. The highly exposed (104) facets provide abundant unsaturated Fe atoms with dangling bonds as nitrogen reduction reaction catalytically active sites. In addition, the NAs architecture enables the enhanced electrochemical surface area (ECSA) to fully manifest the active sites and maintain the mass diffusion. Thus, the selectively exposed (104) facets coupled with the high ECSA of NAs architecture achieve a high FE of 14.89% and a high yield rate of 17.28 μg h^(-1) cm^(-2). This work presents an effective strategy to develop highly efficient catalytic electrodes for electrochemical NRR via facet regulation and nanoarray architecture.展开更多
As one of the most important chemicals and carbon-free energy carriers,ammonia(NH3)has significant energy-related applications in industry and agriculture.Ninety percent of NH_(3) is produced by the Haber-Bosch proces...As one of the most important chemicals and carbon-free energy carriers,ammonia(NH3)has significant energy-related applications in industry and agriculture.Ninety percent of NH_(3) is produced by the Haber-Bosch process using high-purity N_(2) and H_(2) at high temperatures and pressures,which consumes about 1%of the total energy production and causes 1.4% of global CO_(2) emissions.The environmentally friendly electrochemical nitrogen reduction reaction(NRR)with low energy consumption is a promising alternative to the conventional Haber-Bosch process.However,the main issue is the low Faradaic efficiency and NH3 selectivity of electrochemical NRR,caused by inert nitrogen molecules and competitive hydrogen evolution reaction.As one of the cheapest and most abundant transition metals widely utilized in the Haber-Bosch process,the Fe element has presented the potential high performance for the electrochemical NRR.This article summarizes recent advances and research progress in non-noble Fe-based catalysts used for NH_(3) electrosynthesis.Various synthetic protocols,structure/morphology modification,performance improvement,and reaction mechanisms are comprehensively presented.Based on recent experimental and theoretical studies,we aim to illuminate the structure-property relationship and offer an excellent opportunity for engineering advanced Fe-based catalysts for nitrogen fixation.The most critical challenges and opportunities for Fe-based catalysts are also provided.This review would open up a promising avenue toward developing platinum-group-metal-free catalysts for electrochemical NRR applications in the future.展开更多
基金Funded by the National Natural Science Foundation of China (Nos. 22075219 and 51972257)the Fundamental Research Funds for the Central Universities (WUT:2021IA002)the National Key Research Program of China (No. 2016YFA0202602)。
文摘We propose a facile facet regulation enabled by nanoarray architecture to achieve a high faradic efficiency of Fe_(2)O_(3) catalyst for NRR. The a-Fe_(2)O_(3) nanorod arrays (NAs) were directly grown on carbon cloth (CC) with specific (104) facet exposure. The highly exposed (104) facets provide abundant unsaturated Fe atoms with dangling bonds as nitrogen reduction reaction catalytically active sites. In addition, the NAs architecture enables the enhanced electrochemical surface area (ECSA) to fully manifest the active sites and maintain the mass diffusion. Thus, the selectively exposed (104) facets coupled with the high ECSA of NAs architecture achieve a high FE of 14.89% and a high yield rate of 17.28 μg h^(-1) cm^(-2). This work presents an effective strategy to develop highly efficient catalytic electrodes for electrochemical NRR via facet regulation and nanoarray architecture.
基金National Natural Science Foundation of China,Grant/Award Numbers:21902021,21908017Fundamental Research Funds for the Central Universities,Grant/Award Numbers:DUT20RC(4)020,DUT20RC(4)018+1 种基金Open Foundation of Key Laboratory of Industrial Ecology and Environmental Engineering,Grant/Award Numbers:KLIEEE-20-01,KLIEEE-21-02Supercomputing Center of Dalian University of Technology。
文摘As one of the most important chemicals and carbon-free energy carriers,ammonia(NH3)has significant energy-related applications in industry and agriculture.Ninety percent of NH_(3) is produced by the Haber-Bosch process using high-purity N_(2) and H_(2) at high temperatures and pressures,which consumes about 1%of the total energy production and causes 1.4% of global CO_(2) emissions.The environmentally friendly electrochemical nitrogen reduction reaction(NRR)with low energy consumption is a promising alternative to the conventional Haber-Bosch process.However,the main issue is the low Faradaic efficiency and NH3 selectivity of electrochemical NRR,caused by inert nitrogen molecules and competitive hydrogen evolution reaction.As one of the cheapest and most abundant transition metals widely utilized in the Haber-Bosch process,the Fe element has presented the potential high performance for the electrochemical NRR.This article summarizes recent advances and research progress in non-noble Fe-based catalysts used for NH_(3) electrosynthesis.Various synthetic protocols,structure/morphology modification,performance improvement,and reaction mechanisms are comprehensively presented.Based on recent experimental and theoretical studies,we aim to illuminate the structure-property relationship and offer an excellent opportunity for engineering advanced Fe-based catalysts for nitrogen fixation.The most critical challenges and opportunities for Fe-based catalysts are also provided.This review would open up a promising avenue toward developing platinum-group-metal-free catalysts for electrochemical NRR applications in the future.
