Efficient Electroreduction of Nitrate to Ammonia with CuPd Nanoalloy Catalysts

Song，Zhimin1,2; Qin，Lang2; Liu，Yan2; Zhong，Yongzhi2; Guo，Qing1; Geng，Zhigang2; Zeng，Jie2

2023

10.1002/cssc.202300202

ChemSusChem   Impact Factor & Quartile

1864-5631

1864-564X

The electroreduction of nitrate (NO) to valuable ammonia (NH) is a green and appealing alternative to the Haber-Bosch process. Nevertheless, this process suffers from low performance for NH due to the sluggish multi-electron/proton-involved steps. In this work, a CuPd nanoalloy catalyst was developed toward NO electroreduction at ambient conditions. By modulating the atomic ratio of Cu to Pd, the hydrogenation steps of NH synthesis during NO electroreduction can be effectively controlled. At −0.7 V versus reversible hydrogen electrode (vs. RHE), the optimized CuPd electrocatalysts achieved a Faradaic efficiency for NH of 95.5 %, which was 1.3 and 1.8 times higher than that of Cu and Pd, respectively. Notably, at −0.9 V vs. RHE, the CuPd electrocatalysts showed a high yield rate of 36.2 mg h cm for NH with a corresponding partial current density of −430.6 mA cm. Mechanism investigation revealed the enhanced performance originated from the synergistic catalytic cooperation between Cu and Pd sites. The H-atoms adsorbed on the Pd sites prefer to transfer to adjacent nitrogen intermediates adsorbed on the Cu sites, thereby promoting the hydrogenation of intermediates and the formation of NH.

ammonia synthesis CuPd nanoalloys electrocatalysis nitrate electroreduction renewable resources

SCI

English

First ; Corresponding

National Natural Science Foundation of China["92061111","22209161","U19A2015"] ; National Science Fund for Distinguished Young Scholars[21925204] ; National Key Research and Development Program of China["2021YFA1500500","2019YFA0405600"] ; CAS project for young scientists in basic research[YSBR-051] ; K. C. Wong Education[GJTD-2020-15] ; DNL Cooperation Fund, CAS[DNL202003]

Chemistry ; Science & Technology - Other Topics

Chemistry, Multidisciplinary ; Green & Sustainable Science & Technology

WOS:000999322300001

WILEY-V C H VERLAG GMBH

2-s2.0-85160758488

Scopus

1.Department of Chemistry,Southern University of Science and Technology,Shenzhen,Guangdong,518055,China
2.Hefei National Research Center for Physical Sciences at the Microscale,Key Laboratory of Strongly Coupled Quantum Matter Physics of Chinese Academy of Sciences,Key Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education Institutes,Department of Chemical Physics,University of Science and Technology of China,Hefei,Anhui,230026,China

Song，Zhimin,Qin，Lang,Liu，Yan,et al. Efficient Electroreduction of Nitrate to Ammonia with CuPd Nanoalloy Catalysts[J]. ChemSusChem,2023.

Song，Zhimin.,Qin，Lang.,Liu，Yan.,Zhong，Yongzhi.,Guo，Qing.,...&Zeng，Jie.(2023).Efficient Electroreduction of Nitrate to Ammonia with CuPd Nanoalloy Catalysts.ChemSusChem.

Song，Zhimin,et al."Efficient Electroreduction of Nitrate to Ammonia with CuPd Nanoalloy Catalysts".ChemSusChem (2023).