Accelerating Electrocatalytic Nitrate Reduction to Ammonia via Weakening of Intermediate Adsorption on Cu-Based Catalyst  

作　　者：Yizhu Chen Ang Ma Lei Chen Xinyang Liu Yan Li Yan Hong Yushuo Zhang Yunyi Liu Lixin Wei Yudong Li Siqi Li Song Liu 

机构地区：[1]College of Chemistry,Chemical Engineering and Resource Utilization,Northeast Forestry University,Harbin 150040,China [2]School of Physics and Electronic Engineering,Harbin Normal University,Harbin 150025,China [3]Key Laboratory of Bio-Based Material Science and Technology of Ministry of Education,Northeast Forestry University,Harbin 150040,China

出　　处：《Transactions of Tianjin University》2024年第6期488-497,共10页天津大学学报（英文版）

基　　金：This work was financially supported by the National Natural Science Foundation of China(Nos.22208048,22202174,62001097 and 21576238);the Natural Science Foundation of Heilongjiang Province(No.YQ2022B001);We would like to acknowledge the technical support from Analysis and Testing Center of Northeast Forestry University.

摘　　要：Cu-based materials are commonly used in electrocatalytic nitrate reduction reactions(NO 3 RR).NO 3 RR is a“two birds,one stone”approach,simultaneously removing NO 3−pollutants and producing valuable ammonia(NH 3).However,the strong coordination between the NO 3−intermediate and the catalytic active sites seriously hinders the conversion effi ciency.Here,we determined that,through encapsulation strategies,the carbon layer could weaken the NO 3−intermediate binding to active sites,resulting in higher NH 3 yields.We experimentally fabricated electrocatalysts,i.e.,Cu nanoparticles encapsulating(or loaded on)N-doped carbon nanofi bers(NCNFs)called Cu@NCNFs(Cu-NCNFs),using electrostatic spinning.As a result,Cu@NCNFs can achieve NH 3 yields of 17.08 mg/(h·mg cat)at a voltage of−0.84 V and a Faraday effi ciency of 98.15%.Meanwhile,the electrochemical properties of the Cu nanoparticles on the surface of carbon fi bers(Cu-NCNFs)are lower than those of the [e-mail] in situ Raman spectra of Cu@NCNFs and Cu-NCNFs under various reduction potentials during the NO 3 RR process show that catalyst encapsulation within carbon layers can eff ectively reduce the adsorption of N species by the catalyst,thus improving the catalytic performance in the nitrate-to-ammonia catalytic conversion process.

关 键 词：Electrocatalytic nitrate reduction reactions Ammonia synthesis Copper-based electrocatalysts·Electrostatically spun carbon fi ber Regulated adsorption 

分 类 号：TQ113.2[化学工程—无机化工] O643.36[理学—物理化学] X703[理学—化学]