Ruthenium/titanium oxide interface promoted electrochemical nitrogen reduction reaction

被引：15

作者：

Cai, Weizheng ^{[1
]}

Jiang, Ya-Fei ^{[3
]}

Zhang, Jincheng ^{[1
]}

Yang, Hongbin ^{[1
]}

Zhang, Junming ^{[1
]}

Xu, Cong-Qiao ^{[3
]}

Liu, Wei ^{[5
]}

Li, Jun ^{[3
,4
]}

Liu, Bin ^{[1
,2
]}

机构：

[1] Nanyang Technol Univ, Sch Chem & Biomed Engn, Singapore 637459, Singapore

[2] Nanyang Technol Univ, Sch Phys & Math Sci, Div Chem & Biol Chem, 21 Nanyang Link, Singapore 637371, Singapore

[3] Southern Univ Sci & Technol, Dept Chem, Shenzhen 518055, Peoples R China

[4] Tsinghua Univ, Dept Chem, Key Lab Organ Optoelect & Mol Engn, Minist Educ, Beijing 100084, Peoples R China

[5] Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Beijing 116023, Peoples R China

来源：

CHEM CATALYSIS | 2022年 / 2卷 / 07期

基金：

中国国家自然科学基金;

关键词：

SINGLE-CLUSTER CATALYST; AMMONIA-SYNTHESIS; OXYGEN EVOLUTION; N-2; MECHANISM; SPECTRA; WATER; GOLD; XPS;

D O I：

10.1016/j.checat.2022.05.009

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 electrochemical nitrogen reduction reaction ( eNRR) offers a promising strategy to synthesize ammonia at ambient conditions. However, the selectivity and yield of ammonia are greatly impeded by the slow kinetics of the eNRR and the competing hydrogen evolution reaction (HER). Herein, we find that by growing Ru nanoparticles on rutile TiO2, the intimate electronic coupling between Ru nanoparticles and TiO2 support is able to greatly promote the first protonation of N-2 via an associative mechanism in the eNRR while suppressing theHER, resulting in a greatly improved ammonia Faradaic efficiency of 40.7% and yield of 10.4 mgNH3 h(-1) cm(-2) geometric area at -0.15 V versus the reversible hydrogen electrode (RHE) in 0.5 M K2SO4 aqueous solution at room temperature and ambient pressure. Our work provides a general approach to achieve selective electrochemical reaction by controlling the binding strength of reactive intermediates via interface engineering.

引用

页码：1764 / 1774

页数：11

共 46 条

[21] Efficient electrocatalytic nitrogen reduction to ammonia with aqueous silver nanodots [J].

Li, Wenyi ;

Li, Ke ;

Ye, Yixing ;

Zhang, Shengbo ;

Liu, Yanyan ;

Wang, Guozhong ;

Liang, Changhao ;

Zhang, Haimin ;

Zhao, Huijun .

COMMUNICATIONS CHEMISTRY, 2021, 4 (01)

[22] Heterogeneous Fe3 single-cluster catalyst for ammonia synthesis via an associative mechanism [J].

Liu, Jin-Cheng ;

Ma, Xue-Lu ;

Li, Yong ;

Wang, Yang-Gang ;

Xiao, Hai ;

Li, Jun .

NATURE COMMUNICATIONS, 2018, 9

[23]

Lvovich V. F., 2012, Impedance Spectroscopy: Applications to Electrochemical and Dielectric Phenomena, P59, DOI DOI 10.1002/9781118164075.CH5

[24] The significance of electrochemical impedance spectra recorded during active oxygen evolution for oxide covered Ni, Co and Fe electrodes in alkaline solution [J].

Lyons, Michael E. G. ;

Brandon, Michael P. .

JOURNAL OF ELECTROANALYTICAL CHEMISTRY, 2009, 631 (1-2) :62-70

[25] Surface Single-Cluster Catalyst for N2-to-NH3 Thermal Conversion [J].

Ma, Xue-Lu ;

Liu, Jin-Cheng ;

Xiao, Hai ;

Li, Jun .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2018, 140 (01) :46-49

[26] Ammonia synthesis from N2 and H2O using a lithium cycling electrification strategy at atmospheric pressure [J].

McEnaney, Joshua M. ;

Singh, Aayush R. ;

Schwalbe, Jay A. ;

Kibsgaard, Jakob ;

Lin, John C. ;

Cargnello, Matteo ;

Jaramillo, Thomas F. ;

Norskov, Jens K. .

ENERGY & ENVIRONMENTAL SCIENCE, 2017, 10 (07) :1621-1630

[27] Overcoming ammonia synthesis scaling relations with plasma-enabled catalysis [J].

Mehta, Prateek ;

Barboun, Patrick ;

Herrera, Francisco A. ;

Kim, Jongsik ;

Rumbach, Paul ;

Go, David B. ;

Hicks, Jason C. ;

Schneider, William F. .

NATURE CATALYSIS, 2018, 1 (04) :269-275

[28] The Challenge of Electrochemical Ammonia Synthesis: A New Perspective on the Role of Nitrogen Scaling Relations [J].

Montoya, Joseph H. ;

Tsai, Charlie ;

Vojvodic, Aleksandra ;

Norskov, Jens K. .

CHEMSUSCHEM, 2015, 8 (13) :2180-2186

[29] Resolving ruthenium: XPS studies of common ruthenium materials [J].

Morgan, David J. .

SURFACE AND INTERFACE ANALYSIS, 2015, 47 (11) :1072-1079

[30] Promoting Effects of Lanthan on Ru/AC for Ammonia Synthesis: Tuning Catalytic Efficiency and Stability Simultaneously [J].

Ni, Jun ;

Lin, Jingdong ;

Wang, Xiuyun ;

Lin, Bingyu ;

Lin, Jianxin ;

Jiang, Lilong .

CHEMISTRYSELECT, 2017, 2 (21) :6040-6046

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