Three-Dimensional Porous Cu/Cu2+1O Nanosheet Arrays Promote Electrochemical Nitrate-to-Ammonia Conversion

被引：10

作者：

Sun, Chaozhong ^{[1
]}

Xiao, Yingguan ^{[1
]}

Liu, Xiang ^{[2
]}

Hu, Jie ^{[1
]}

Zhao, Qing ^{[1
]}

Yin, Zhengliang ^{[1
]}

Cao, Shunsheng ^{[1
]}

机构：

[1] Jiangsu Univ, Sch Mat Sci & Engn, Zhenjiang 212013, Peoples R China

[2] Zhenjiang Coll, Jiangsu Higher Vocat Coll Engn Res Ctr Green Energ, Zhenjiang 212028, Peoples R China

来源：

INORGANIC CHEMISTRY | 2024年 / 63卷 / 25期

基金：

中国国家自然科学基金;

关键词：

CU; NANOPARTICLES; REDUCTION; DRIVEN;

D O I：

10.1021/acs.inorgchem.4c01737

中图分类号：

O61 [无机化学];

学科分类号：

070301 ; 081704 ;

摘要：

The efficiency of electrochemical nitrate (NO3-) reduction to ammonia (NH3) still remains a challenge due to the sluggish kinetics of the complex eight-electron reduction process and competitive hydrogen evolution reaction (HER). Herein, we designed new three-dimensional (3D) porous Cu/Cu2+1O nanosheet arrays (Cu/Cu2+1O NSA) by coupling a template-directed method with in situ electroreduction. Thanks to the 3D porous structure and in-plane heterojunctions, Cu/Cu2+1O NSA can provide abundant active sites and a good interfacial effect, obtaining the maximum Faradaic efficiency (FE) of ammonia (88.09%) and high yield rate of 0.2634 mmol h(-1) cm(-2), which is higher than that of CuO nanosheets (77.81% and 0.2188 mmol h(-1) cm(-2)) and CuO nanoparticles (34.60% and 0.0692 mmol h(-1) cm(-2)). Experimental results and DFT simulations show that the interface effect of Cu/Cu2+1O can decrease the reaction energy barrier of the key step (*NO to *NOH) and can greatly inhibit the competitive hydrogen evolution reaction, thereby achieving excellent electrocatalytic performance for nitrate-to-ammonia conversion.

引用

页码：11852 / 11859

页数：8

共 46 条

[1] Electrical Pulse-Driven Periodic Self-Repair of Cu-Ni Tandem Catalyst for Efficient Ammonia Synthesis from Nitrate [J].

Bu, Yongguang ;

Wang, Chao ;

Zhang, Wenkai ;

Yang, Xiaohan ;

Ding, Jie ;

Gao, Guandao .

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2023, 62 (24)

[2] Interfacial hydrogen bonding-involved electrocatalytic ammonia synthesis on OH-terminated MXene [J].

Cai, Jinmeng ;

Huang, Jingjing ;

Cao, Ang ;

Wei, Yingying ;

Wang, Huimin ;

Li, Xue ;

Jiang, Zheng ;

Waterhouse, Geoffrey I. N. ;

Lu, Siyu ;

Zang, Shang-Quan .

APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY, 2023, 328

[3] One-pot synthesis of porous TiO2/BiOI adsorbent with high removal efficiency and excellent recyclability towards tetracyclines [J].

Chen, Juanrong ;

He, Jie ;

Yin, Zhengliang ;

Wang, Tingwei ;

Liu, Shunan ;

Cao, Shunsheng .

CERAMICS INTERNATIONAL, 2023, 49 (13) :22139-22148

[4] Cation Substitution Strategy for Developing Perovskite Oxide with Rich Oxygen Vacancy-Mediated Charge Redistribution Enables Highly Efficient Nitrate Electroreduction to Ammonia [J].

Chu, Kaibin ;

Zong, Wei ;

Xue, Guohao ;

Guo, Hele ;

Qin, Jingjing ;

Zhu, Haiyan ;

Zhang, Nan ;

Tian, Zhihong ;

Dong, Hongliang ;

Miao, Yue-E. ;

Roeffaers, Maarten B. J. ;

Hofkens, Johan ;

Lai, Feili ;

Liu, Tianxi .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2023, 145 (39) :21387-21396

[5] Interfacially Engineered Nanoporous Cu/MnOx Hybrids for Highly Efficient Electrochemical Ammonia Synthesis via Nitrate Reduction [J].

Cui, Yuhuan ;

Dong, Anqi ;

Zhou, Yitong ;

Qu, Yanbin ;

Zhao, Ming ;

Wang, Zhili ;

Jiang, Qing .

SMALL, 2023, 19 (17)

[6] Durable Electrocatalytic Reduction of Nitrate to Ammonia over Defective Pseudobrookite Fe2TiO5 Nanofibers with Abundant Oxygen Vacancies [J].

Du, Hongting ;

Guo, Haoran ;

Wang, Kaike ;

Du, Xiangning ;

Beshiwork, Bayu Admasu ;

Sun, Shengjun ;

Luo, Yongsong ;

Liu, Qian ;

Li, Tingshuai ;

Sun, Xuping .

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2023, 62 (05)

[7] Active hydrogen boosts electrochemical nitrate reduction to ammonia [J].

Fan, Kui ;

Xie, Wenfu ;

Li, Jinze ;

Sun, Yining ;

Xu, Pengcheng ;

Tang, Yang ;

Li, Zhenhua ;

Shao, Mingfei .

NATURE COMMUNICATIONS, 2022, 13 (01)

[8] Boosting nitrate electroreduction to ammonia via in situ generated stacking faults in oxide-derived copper [J].

Fang, Ling ;

Wang, Sha ;

Song, Cheng ;

Lu, Shun ;

Yang, Xiaohui ;

Qi, Xueqiang ;

Liu, Hong .

CHEMICAL ENGINEERING JOURNAL, 2022, 446

[9] Tuning mobility of intermediate and electron transfer to enhance electrochemical reduction of nitrate to ammonia on Cu2O/Cu interface [J].

Fu, Wenyang ;

Hu, Zhongzheng ;

Zheng, Yang ;

Su, Pei ;

Zhang, Qizhan ;

Jiao, Yongli ;

Zhou, Minghua .

CHEMICAL ENGINEERING JOURNAL, 2022, 433

[10] Enhancing Electrochemical Nitrate Reduction to Ammonia over Cu Nanosheets via Facet Tandem Catalysis [J].

Fu, Yunfan ;

Wang, Shuo ;

Wang, Yi ;

Wei, Pengfei ;

Shao, Jiaqi ;

Liu, Tianfu ;

Wang, Guoxiong ;

Bao, Xinhe .

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2023, 62 (26)

← 1 2 3 4 5 →