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Electron-deficient Cu delta+ stabilized by interfacial Cu-O-Al bonding for accelerating electrocatalytic nitrate conversion

文献类型：期刊论文

作者Jiang, Guangming2; Peng, Min2; Hu, Lin2; Ouyang, Jiayi2; Lv, Xiaoshu2; Yang, Zhehan2; Liang, Xinyuan2; Liu, Yuan1; Liu, Hong1
刊名CHEMICAL ENGINEERING JOURNAL
出版日期2022-05-01
卷号435页码:9
关键词Nitrate reduction Electrocatalysis Copper Selectivity Metal-support interactions
ISSN号1385-8947
DOI10.1016/j.cej.2022.134853
通讯作者Jiang, Guangming(jiangguangming@zju.edu.cn) ; Liu, Hong(liuhong@cigit.ac.cn)
英文摘要Electrocatalytic nitrate reduction to NH3 not only enables the recycling of nutrients from nitrate wastewater but can also lead to complete nitrogen elimination when paired with an NH3 oxidation reaction to achieve innocuous N-2. Albeit electron-deficient copper (Cu delta+) is an active catalytic site for an electrocatalytic nitrate reduction reaction (ENRR), its stabilization under the reductive polarization potential of ENRR is challenging. Herein, we report the in-situ electroreduction of CuAl-mixed oxide to construct a Cu-Al2O3 interface with strong metal-support interactions (CuAl-LDO-r), which can form and stabilize Cu delta+ via Cu-O-Al bonds. The batch ENRR tests revealed that Cu52Al48-LDO-r delivers an NH3-N selectivity of 97.4%, stable specific activity of 661.6 mg-N m(-2)h(-1) for NH3-N production (faradaic current efficiency of 70.4%), and minimal Cu leaching when reducing 22.5 mg L-1 NO3--N at 1.10 V vs. Ag/AgCl, outperforming most of the reported catalysts under similar reaction conditions. Combined in-situ spectrometric analyses and theoretical calculations demonstrate that the robust performance of Cu delta+ originates from its substantial affinity toward the N-intermediates, which promotes molecule activation and prevents intercoupling to dinitrogen species. For nitrate elimination, the ENRR was coupled with an anode-driven breakpoint chlorination reaction, and the designed system enabled complete conversion of NO3--N (44.5 mg L-1) to N-2 with an electrical consumption of 1.82 kwh mol(N)(-1).
资助项目National Natural Science Foundation of China[22176019] ; National Natural Science Foundation of China[51978110] ; National Natural Science Foundation of China[21804014] ; Natural Science Foundation of Chongqing Science & Technology Com-mission[cstc2019jcyj-msxmX0260] ; Science and Technology Research Program of Chongqing Municipal Education Commission[KJQN201800829] ; Science and Technology Research Program of Chongqing Municipal Education Commission[KJQN201900837] ; Science and Technology Research Program of Chongqing Municipal Education Commission[K202000802]
WOS研究方向Engineering
语种英语
WOS记录号WOS:000773616600004
出版者ELSEVIER SCIENCE SA
源URL[http://119.78.100.138/handle/2HOD01W0/15846]  
专题中国科学院重庆绿色智能技术研究院
通讯作者Jiang, Guangming; Liu, Hong
作者单位1.Chinese Acad Sci, Chongqing Inst Green & Intelligent Technol, 266 Fangzheng Ave, Chongqing 400714, Peoples R China
2.Chongqing Technol & Business Univ, Engn Res Ctr Waste Oil Recovery Technol & Equipme, Minist Educ, Chongqing 400067, Peoples R China
推荐引用方式
GB/T 7714		 Jiang, Guangming,Peng, Min,Hu, Lin,et al. Electron-deficient Cu delta+ stabilized by interfacial Cu-O-Al bonding for accelerating electrocatalytic nitrate conversion[J]. CHEMICAL ENGINEERING JOURNAL,2022,435:9.
APA Jiang, Guangming.,Peng, Min.,Hu, Lin.,Ouyang, Jiayi.,Lv, Xiaoshu.,...&Liu, Hong.(2022).Electron-deficient Cu delta+ stabilized by interfacial Cu-O-Al bonding for accelerating electrocatalytic nitrate conversion.CHEMICAL ENGINEERING JOURNAL,435,9.
MLA Jiang, Guangming,et al."Electron-deficient Cu delta+ stabilized by interfacial Cu-O-Al bonding for accelerating electrocatalytic nitrate conversion".CHEMICAL ENGINEERING JOURNAL 435(2022):9.

入库方式： OAI收割

来源：重庆绿色智能技术研究院

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