High-Performance Electrochemical NO Reduction into NH3 by MoS2 Nanosheet

被引:221
|
作者
Zhang, Longcheng [1 ,2 ]
Liang, Jie [1 ]
Wang, Yuanyuan [3 ,4 ]
Mou, Ting [1 ]
Lin, Yiting [1 ]
Yue, Luchao [1 ,2 ]
Li, Tingshuai [1 ]
Liu, Qian [5 ]
Luo, Yonglan [5 ]
Li, Na [6 ]
Tang, Bo [6 ]
Liu, Yang [7 ]
Gao, Shuyan [7 ]
Alshehri, Abdulmohsen Ali [8 ]
Guo, Xiaodong [2 ]
Ma, Dongwei [3 ,4 ]
Sun, Xuping [1 ]
机构
[1] Univ Elect Sci & Technol China, Inst Fundamental & Frontier Sci, Chengdu 610054, Sichuan, Peoples R China
[2] Sichuan Univ, Sch Chem Engn, Chengdu 610065, Sichuan, Peoples R China
[3] Henan Univ, Key Lab Special Funct Mat, Minist Educ, Kaifeng 475004, Henan, Peoples R China
[4] Henan Univ, Sch Mat Sci & Engn, Kaifeng 475004, Henan, Peoples R China
[5] Chengdu Univ, Inst Adv Study, Chengdu 610106, Sichuan, Peoples R China
[6] Shandong Normal Univ, Coll Chem Chem Engn & Mat Sci, Jinan 250014, Shandong, Peoples R China
[7] Henan Normal Univ, Sch Mat Sci & Engn, Xinxiang 453007, Henan, Peoples R China
[8] King Abdulaziz Univ, Fac Sci, Chem Dept, POB 80203, Jeddah 21589, Saudi Arabia
基金
中国国家自然科学基金;
关键词
density functional theory; electrocatalysis; MoS2; NH3; synthesis; NO reduction reaction; ELECTROCATALYTIC NITROGEN REDUCTION; NITRIC-OXIDE; AMMONIA; GRAPHDIYNE; CHEMISTRY; CATALYSIS; REMOVAL; DESIGN;
D O I
10.1002/anie.202110879
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Electrochemical reduction of NO not only offers an attractive alternative to the Haber-Bosch process for ambient NH3 production but mitigates the human-caused unbalance of nitrogen cycle. Herein, we report that MoS2 nanosheet on graphite felt (MoS2/GF) acts as an efficient and robust 3D electrocatalyst for NO-to-NH3 conversion. In acidic electrolyte, such MoS2/GF attains a maximal Faradaic efficiency of 76.6 % and a large NH3 yield of up to 99.6 mu mol cm(-2) h(-1). Using MoS2 nanosheet-loaded carbon paper as the cathode, a proof-of-concept device of Zn-NO battery was assembled to deliver a discharge power density of 1.04 mW cm(-2) and an NH3 yield of 411.8 mu g h(-1) mg(cat.)(-1). Calculations reveal that the positively charged Mo-edge sites facilitate NO adsorption/activation via an acceptance-donation mechanism and disfavor the binding of protons and the coupling of N-N bond.
引用
收藏
页码:25263 / 25268
页数:6
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