Copper single-atom catalyst as a high-performance electrocatalyst for nitrate-ammonium conversion

Chen，Huihuang1,2; Zhang，Chunqing1; Sheng，Li2; Wang，Miaomiao3; Fu，Weng4; Gao，Shuai4; Zhang，Zhirong2; Chen，Shaoqing5; Si，Rui3; Wang，Lianzhou4; Yang，Bo1

2022-07-15

10.1016/j.jhazmat.2022.128892

JOURNAL OF HAZARDOUS MATERIALS   影响因子和分区

0304-3894

1873-3336

Electrocatalytic nitrate reduction reaction (NORR), as a promising alternative to the Haber-Bosh process, provides new opportunities for ammonia (NH) production from the environmental and energy viewpoint. However, the NH yield rate and selectivity for NORR are still limited due to the lack of efficient electrocatalysts. Herein, we demonstrate an active and selective copper single-atom catalyst (Cu-N-C) for nitrate reduction to NH. The complete conversion of nitrate (50 mg L NO-N) was achieved at −1.5 V vs. SCE with a high NH yield rate (9.23 mg h mg ) and selectivity (94%). Remarkably, Cu-N-C dramatically inhibited the formation of toxic nitrite and double-nitrogen products due to the enhanced nitrite adsorption and restrained N-N coupling that led to nitrate deep reduction to NH. The remaining nitrate (0.06 mg L) and nitrite (1 mg L) fully meet the drinking-water standards. Density functional theory simulations reveal that the single-site nature of Cu-N-C facilitated the reduction of HNO* to NO* and NH* to NH, thus leading to the selective nitrate reduction to NH.

15N isotope labelling 1H NMR Electrocatalysis Nitrate reduction Reaction pathway

SCI ; EI

英语

其他

National Natural Science Foundation of China[22005288,22176131]

Engineering ; Environmental Sciences & Ecology

Engineering, Environmental ; Environmental Sciences

WOS:000793535400002

ELSEVIER

20221712008900

Ammonia ; Copper ; Copper compounds ; Density functional theory ; Electrocatalysts ; Nitrates ; Potable water

Water Resources:444 ; Copper:544.1 ; Electrochemistry:801.4.1 ; Chemical Reactions:802.2 ; Chemical Agents and Basic Industrial Chemicals:803 ; Inorganic Compounds:804.2 ; Probability Theory:922.1 ; Atomic and Molecular Physics:931.3 ; Quantum Theory; Quantum Mechanics:931.4

ENGINEERING

2-s2.0-85128486390

Scopus

1.College of Chemistry and Environmental Engineering,Shenzhen University,Shenzhen,518060,China
2.National Synchrotron Radiation Laboratory,Hefei National Laboratory for Physical Sciences at the Microscale,University of Science and Technology of China,Hefei,230026,China
3.Shanghai Synchrotron Radiation Facility,Shanghai Institute of Applied Physics,Chinese Academy of Sciences,Shanghai,201204,China
4.School of Chemical Engineering,The University of Queensland,Brisbane,4072,Australia
5.Department of Materials Science and Engineering,Southern University of Science and Technology,Shenzhen,518055,China

Chen，Huihuang,Zhang，Chunqing,Sheng，Li,et al. Copper single-atom catalyst as a high-performance electrocatalyst for nitrate-ammonium conversion[J]. JOURNAL OF HAZARDOUS MATERIALS,2022,434.

Chen，Huihuang.,Zhang，Chunqing.,Sheng，Li.,Wang，Miaomiao.,Fu，Weng.,...&Yang，Bo.(2022).Copper single-atom catalyst as a high-performance electrocatalyst for nitrate-ammonium conversion.JOURNAL OF HAZARDOUS MATERIALS,434.

Chen，Huihuang,et al."Copper single-atom catalyst as a high-performance electrocatalyst for nitrate-ammonium conversion".JOURNAL OF HAZARDOUS MATERIALS 434(2022).