Boron-Doped TiO2 for Efficient Electrocatalytic N2 Fixation to NH3 at Ambient Conditions

被引：124

作者：

Wang, Yuan ^{[1
,2
]}

Jia, Kun ^{[1
,2
]}

Pan, Qi ^{[1
,2
]}

Xu, Yadi ^{[1
]}

Liu, Qian ^{[3
]}

Cui, Guanwei ^{[4
]}

Guo, Xiaodong ^{[1
]}

Sun, Xuping ^{[2
]}

机构：

[1] Sichuan Univ, Inst Chem Engn, Chengdu 610065, Sichuan, Peoples R China

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

[3] Univ Elect Sci & Technol China, Sch Mat & Energy, Chengdu 611731, Sichuan, Peoples R China

[4] Shandong Normal Univ, Coll Chem Chem Engn & Mat Sci, Jinan 250014, Shandong, Peoples R China

来源：

ACS SUSTAINABLE CHEMISTRY & ENGINEERING | 2019年 / 7卷 / 01期

基金：

中国国家自然科学基金;

关键词：

TiO2; B Doping; N-2 Reduction reaction; NH3; Synthesis; Ambient conditions; ANATASE TIO2; ATMOSPHERIC-PRESSURE; AMMONIA-SYNTHESIS; NANOTUBE ARRAY; NITROGEN; TEMPERATURE; REDUCTION; WATER; ELECTROSYNTHESIS; NANOPARTICLES;

D O I：

10.1021/acssuschemeng.8b05332

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

NH3 synthesis almost relies on the energy-intensive Haber-Bosch process with abandoned CO2 emission. Electrochemical N-2 reduction offers an environmentally friendly process for sustainable artificial N-2 fixation at ambient conditions, but stable and efficient catalysts are demanded for the N-2 reduction reaction (NRR). In this Letter, we report that boron-doped TiO2 acts as an efficient non-noble-metal NRR catalyst for electrochemical N-2 reduction to NH3 at ambient conditions. This catalyst delivers remarkable NRR performance in 0.1 M Na2SO4 with a NH3 yield of 14.4 mu g.h(-1).mg(cat)(-1). and a Faradaic efficiency of 3.4% at -0.8 V vs reversible hydrogen electrode. Notably, it is also excellent in electrochemical durability and selectivity for NH3 formation.

引用

页码：117 / 122

页数：11

共 50 条

[1] Light-driven dinitrogen reduction catalyzed by a CdS:nitrogenase MoFe protein biohybrid [J].

Brown, Katherine A. ;

Harris, Derek F. ;

Wilker, Molly B. ;

Rasmussen, Andrew ;

Khadka, Nimesh ;

Hamby, Hayden ;

Keable, Stephen ;

Dukovic, Gordana ;

Peters, John W. ;

Seefeldt, Lance C. ;

King, Paul W. .

SCIENCE, 2016, 352 (6284) :448-450

[2] Electrocatalytic Synthesis of Ammonia at Room Temperature and Atmospheric Pressure from Water and Nitrogen on a Carbon-Nanotube-Based Electrocatalyst [J].

Chen, Shiming ;

Perathoner, Siglinda ;

Ampelli, Claudio ;

Mebrahtu, Chalachew ;

Su, Dangsheng ;

Centi, Gabriele .

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2017, 56 (10) :2699-2703

[3] One electron at a time [J].

Chirik, Paul J. .

NATURE CHEMISTRY, 2009, 1 (07) :520-522

[4]

Dybkjaer I., 1995, AMMONIA, P199, DOI DOI 10.1007/978-3-642-79197-0_6

[5] Boron Environments in B-Doped and (B, N)-Codoped TiO2 Photocatalysts: A Combined Solid-State NMR and Theoretical Calculation Study [J].

Feng, Ningdong ;

Zheng, Anmin ;

Wang, Qiang ;

Ren, Pingping ;

Gao, Xiuzhi ;

Liu, Shang-Bin ;

Shen, Zhurui ;

Chen, Tiehong ;

Deng, Feng .

JOURNAL OF PHYSICAL CHEMISTRY C, 2011, 115 (06) :2709-2719

[6] Boron-Doped Anatase TiO2: Pure and Hybrid DFT Calculations [J].

Finazzi, Emanuele ;

Di Valentin, Cristiana ;

Pacchioni, Gianfranco .

JOURNAL OF PHYSICAL CHEMISTRY C, 2009, 113 (01) :220-228

[7] Chemical state and environment of boron dopant in B,N-codoped anatase TiO2 nanoparticles:: An avenue for probing diamagnetic dopants in TiO2 by electron paramagnetic resonance spectroscopy [J].

Gopal, Neeruganti O. ;

Lo, Hsin-Hsi ;

Ke, Shyue-Chu .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2008, 130 (09) :2760-+

[8] Rational design of electrocatalysts and photo(electro) catalysts for nitrogen reduction to ammonia (NH3) under ambient conditions [J].

Guo, Chunxian ;

Ran, Jingrun ;

Vasileff, Anthony ;

Qiao, Shi-Zhang .

ENERGY & ENVIRONMENTAL SCIENCE, 2018, 11 (01) :45-56

[9] Ambient N2 fixation to NH3 at ambient conditions: Using Nb2O5 nanofiber as a high-performance electrocatalyst [J].

Han, Jingrui ;

Liu, Zaichun ;

Ma, Yongjun ;

Cui, Guanwei ;

Xie, Fengyu ;

Wang, Faxing ;

Wu, Yuping ;

Gao, Shuyan ;

Xu, Yuanhong ;

Sun, Xuping .

NANO ENERGY, 2018, 52 :264-270

[10] MoO3 nanosheets for efficient electrocatalytic N2 fixation to NH3 [J].

Han, Jingrui ;

Ji, Xuqiang ;

Ren, Xiang ;

Cui, Guanwei ;

Li, Lei ;

Xie, Fengyu ;

Wang, Hui ;

Li, Baihai ;

Sun, Xuping .

JOURNAL OF MATERIALS CHEMISTRY A, 2018, 6 (27) :12974-12977

← 1 2 3 4 5 →