Boron Nanosheet: An Elemental Two-Dimensional (2D) Material for Ambient Electrocatalytic N2-to-NH3 Fixation in Neutral Media

被引：275

作者：

Zhang, Xiaoxue ^{[1
]}

Wu, Tongwei ^{[3
]}

Wang, Huanbo ^{[2
]}

Zhao, Runbo ^{[3
]}

Chen, Hongyu ^{[1
,3
]}

Wang, Ting ^{[1
,3
]}

Wei, Peipei ^{[3
]}

Luo, Yonglan ^{[1
]}

Zhang, Yanning ^{[3
]}

Sun, Xuping ^{[1
,3
]}

机构：

[1] China West Normal Univ, Coll Chem & Chem Engn, Chem Synth & Pollut Control Key Lab Sichuan Prov, Nanchong 637002, Sichuan, Peoples R China

[2] Southwest Univ Sci & Technol, Sch Environm & Resource, Mianyang 621010, Sichuan, Peoples R China

[3] Univ Elect Sci & Technol China, Inst Fundamental & Frontier Sci, Chengdu 610054, Sichuan, Peoples R China

来源：

ACS CATALYSIS | 2019年 / 9卷 / 05期

关键词：

boron nanosheet; elemental 2D material; N-2 reduction reaction; neutral electrolyte; density functional theory calculations; ATMOSPHERIC-PRESSURE; ELECTROCHEMICAL SYNTHESIS; LOW-TEMPERATURE; N-2; FIXATION; NITROGEN; AMMONIA; NH3; REDUCTION; GRAPHENE; WATER;

D O I：

10.1021/acscatal.8b05134

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

The Haber-Bosch process for industrial NH3 production suffers from harsh reaction conditions and serious CO2 emission. Electrochemical N-2 reduction offers a carbon-neutral alternative for more energy-saving NH3 synthesis but requires active electrocatalysts for the N-2 reduction reaction (NRR). In this Letter, boron nanosheet (BNS) is proposed as an elemental two-dimensional (2D) material to effectively catalyze the NRR toward NH3 synthesis with excellent selectivity. When tested in 0.1 M Na2SO4, such BNS catalyst attains a high Faradaic efficiency of 4.04% and a large NH3 yield of 13.22 mu g h(-1) mg(cat)(-1) at -0.80 V vs reversible hydrogen electrode, with strong electrochemical durability. Density functional theory calculations suggest that the B atoms of both oxidized and H-deactivated BNS can catalyze the NRR more effectively than clean BNS, and the rate-determining step is the desorption process of the second NH3 gas.

引用

页码：4609 / 4615

页数：13

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