Boosting Electrocatalytic Ammonia Production through Mimicking "π Back-Donation"

被引：126

作者：

Lv, Chade ^{[1
]}

Zhong, Lixiang ^{[1
]}

Yao, Yao ^{[3
]}

Liu, Daobin ^{[4
]}

Kong, Yi ^{[5
]}

Jin, Xiaoli ^{[6
]}

Fang, Zhiwei ^{[2
]}

Xu, Wenjie ^{[4
]}

Yan, Chunshuang ^{[1
]}

Khang Ngoc Dinh ^{[1
]}

Shao, Minhua ^{[3
]}

Song, Li ^{[4
]}

Chen, Gang ^{[5
]}

Li, Shuzhou ^{[1
]}

Yan, Qingyu ^{[1
]}

Yu, Guihua ^{[2
]}

机构：

[1] Nanyang Technol Univ, Sch Mat Sci & Engn, Singapore 639798, Singapore

[2] Univ Texas Austin, Texas Mat Inst, Mat Sci & Engn Program, Austin, TX 78712 USA

[3] Hong Kong Univ Sci & Technol, Dept Chem & Biol Engn, Hong Kong, Peoples R China

[4] Univ Sci & Technol China, CAS Ctr Excellence Nanosci, Natl Synchrotron Radiat Lab, Hefei 230029, Anhui, Peoples R China

[5] Harbin Inst Technol, Sch Chem & Chem Engn, MIIT Key Lab Crit Mat Technol New Energy Convers, Harbin 150001, Heilongjiang, Peoples R China

[6] Nanyang Normal Univ, Coll Chem & Pharmaceut Engn, Engn Technol Res Ctr Henan Prov Solar Catalysis, Nanyang 473061, Henan, Peoples R China

来源：

CHEM | 2020年 / 6卷 / 10期

关键词：

N-2; FIXATION; REDUCTION REACTION; NITROGEN-FIXATION; ELECTROREDUCTION; TEMPERATURE; PERFORMANCE; NANOSHEET; OXIDE;

D O I：

10.1016/j.chempr.2020.07.006

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

Electrocatalytic dinitrogen reduction reaction (N2RR) is an emerging route for ammonia synthesis at ambient conditions. Albeit the "pi back-donation" process enables N2RR activity on transition metals with empty d-orbitals, given its dilemma in overcoming hydrogen evolution reaction (HER) competition, exploring p-block-element. based catalysts with relatively inferior HER activity is achievable for high selectivity. The challenge lies in designing rational structure to improve N2RR activity. Here, we synergistically integrate oxygen vacancy (V-O) with hydroxyl on Bi4O5I2 (V-O-Bi4O5I2 -OH), which render this p-block-element-based material active to mimic "Tr back-donation" behavior because of sufficient vacant orbitals. In neutral media, the electrocatalytic N2RR performance of V-O-Bi4O5I2 -OH in terms of splendid faradic efficiency (32.4%) is superior to most of the prior reports using p-block-element-based catalysts. Our findings show a new strategy toward standout N2RR activity, which holds great potential in exploiting other p-block-element-based electrocatalysts.

引用

页码：2690 / 2702

页数：13

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