Synergistically enhancing nitrate reduction into N_(2)in water by N-doped Pd-Cu biochar bimetallic single-atom electrocatalysis  

作　　者：Lihao Zhang Yuqing Wu Zongqiang Zhu Yinian Zhu Yi Dong Meina Liang Huan Deng 

机构地区：[1]College of Environmental Science and Engineering,Guilin University of Technology,Guilin 541006,People’s Republic of China. [2]Guangxi Key Laboratory of Environmental Pollution Control Theory and Technology,Guilin 541006,People’s Republic of China. [3]Collaborative Innovation Center for Water Pollution Control and Water Safety in Karst Area,Guilin University of Technology,Guilin 541006,People’s Republic of China [4]Key Laboratory of Drinking Water Science and Technology,Research Center for Eco-Environmental Sciences,Chinese Academy of Sciences,Beijing 100035,People’s Republic of China.

出　　处：《Biochar》2024年第1期114-131,共18页生物炭(英文)

基　　金：supported by the National Natural Science Foundation of China(Nos.51978188,42063003,52160017);the Chinese Postdoctoral Science Foundation(2019M650869);the Research Foundation of Guangxi Key Laboratory of Environmental Pollution Control Theory and Technology(Guikeneng 2301Z001);the Special Fundation for Guangxi Distinguished Experts and Program for High Level Innovation Team and Outstanding Scholar of Universities in Guangxi(GuiCaiJiaoHan[2018]319).

摘　　要：Noble metal materials have been identified as high efficiency catalysts for electrocatalytic reduction of nitrate,and the synthesis and manufacture of high catalytic activity and environmentally friendly catalysts of activating hydrogen for water purification applications is extremely attractive.In this work,the Pd-Cu single-atom catalysts(Pd-Cu-N-BC)were first prepared by direct growth of Pd-Cu single-atom on bamboo biochar by regulating the concentration of precursors and doping method,and then enhanced electrocatalytic reduction nitrate performance and N2 gen-eration.The results showed that Pd-Cu-N-BC displayed excellent catalytic activity and reusability in electrocatalytic reduction nitrate with a low potential of 0.47 V vs.RHE(@10 mA cm−2).The maximum nitrate removal efficiency and N2 generation could reach about 100%and 72.32%within 180 min,respectively.The density functional theory(DFT)calculations confirmed that Cu atoms could catalyze the electrochemical reduction of nitrate to nitrite,and Pd atoms anchored in the nitrogen-doped biochar(N-BC)lattice could catalyze electrochemical reduction of nitrite to N2 involving the formation of hydrogen radical(H*).The characterization results of XANES showed that electronic synergistic effect between Pd and Cu single atoms significantly promotes the N2 production through hydrogenation while inhibiting the generation of byproducts,leading to significantly enhanced electrocatalytic reduction of nitrate to N2.Finally,Pd-Cu-N-BC was designed as a 3D particle electrode for enhanced electrocatalytic reduction of nitrate,exhibiting excellent stability and reusability,which could be considered as a suitable candidate for applications in the remediation of nitrate contamination.

关 键 词：Bamboo biochar Single atom catalyst Electrocatalytic denitration Hydrogen evolution reaction Density functional theory 

分 类 号：O64[理学—物理化学]