The electrochemical reduction of nitrate to ammonia(NH3) can be used to recycle nitrogen and offers a decarbonized route for sustainable NH3production,but requires efficient electrocatalysts.Herein,we have rationally ...The electrochemical reduction of nitrate to ammonia(NH3) can be used to recycle nitrogen and offers a decarbonized route for sustainable NH3production,but requires efficient electrocatalysts.Herein,we have rationally designed and fabricated a novel self-supported electrocatalyst comprised of Ni nanoparticles(NiNPs) embedded in Ni single atoms(NiSAs) anchored to nitrogen-doped carbon nanotubes grown on carbon cloth(NiNPs@NiSAs-NCNTs/CC) used for an efficient nitrate reduction reaction(NO3-RR) to produce NH_(3).The electrocatalyst can attain a maximum NH3yield rate of 27.67±1.16 mgNH3h^(-1)cm^(-2)at-1.4 V vs.reversible hydrogen electrode(RHE) and nearly 100% Faradic efficiency in the range of-1.2--1.4 V vs.RHE in a neutral medium,outperforming the previously reported Ni-based catalysts.Our experimental analysis and theoretical calculations have demonstrated that the moderate electrondeficient state of NiSAsregulated by NiNPsnot only facilitates the enrichment of NO_(3)^(-),but also benefits the formation of NO3*and decrease in the energy barrier of the rate-limiting step,thus resulting in the enhanced NO3-RR performance.展开更多
基金supported by the National Natural Science Foundation of China(21971129, 21961022, 21661023, 22172083, and 21962013)the Inner Mongolia Autonomous Region 2022 Leading Talent Team of Science and Technology (2022LJRC0008)+8 种基金the Natural Science Foundation of Inner Mongolia Autonomous Region of China(2022BS02014 and 2021BS02007)the 111 Project (D20033)the Natural Science Foundation of Inner Mongolia Autonomous Region of China (2021JQ02)the Program for Innovative Research Team in Universities of Inner Mongolia Autonomous Region (NJYT23031)the Program of Higher-level Talents of IMU (21300-5215101)the“Grassland Leading Talent” Program of Inner Mongoliathe“Grassland Talent” Innovation Team of Inner Mongoliathe“Science and Technology for a Better Development of Inner Mongolia” Program(2020XM03)the Science and Technology Project of Ordos(2021 ZDI 11-14)。
文摘The electrochemical reduction of nitrate to ammonia(NH3) can be used to recycle nitrogen and offers a decarbonized route for sustainable NH3production,but requires efficient electrocatalysts.Herein,we have rationally designed and fabricated a novel self-supported electrocatalyst comprised of Ni nanoparticles(NiNPs) embedded in Ni single atoms(NiSAs) anchored to nitrogen-doped carbon nanotubes grown on carbon cloth(NiNPs@NiSAs-NCNTs/CC) used for an efficient nitrate reduction reaction(NO3-RR) to produce NH_(3).The electrocatalyst can attain a maximum NH3yield rate of 27.67±1.16 mgNH3h^(-1)cm^(-2)at-1.4 V vs.reversible hydrogen electrode(RHE) and nearly 100% Faradic efficiency in the range of-1.2--1.4 V vs.RHE in a neutral medium,outperforming the previously reported Ni-based catalysts.Our experimental analysis and theoretical calculations have demonstrated that the moderate electrondeficient state of NiSAsregulated by NiNPsnot only facilitates the enrichment of NO_(3)^(-),but also benefits the formation of NO3*and decrease in the energy barrier of the rate-limiting step,thus resulting in the enhanced NO3-RR performance.
