Molecular electrocatalysts for rapid and selective reduction of nitrogenous waste to ammonia

Jiang，Zhan1; Wang，Yamin2; Lin，Zhicao1; Yuan，Yubo1; Zhang，Xiao3; Tang，Yirong1; Wang，Hongxuan1; Li，Huan1; Jin，Chuyao3; Liang，Yongye1,4

2023

10.1039/d2ee03502b

Energy and Environmental Science   Impact Factor & Quartile

1754-5692

1754-5706

Electrocatalysis of the nitrate (NO) reduction reaction (NORR) or nitrite (NO) reduction reaction (NORR) is a sustainable route for removing nitrogenous pollutes and producing ammonia (NH). Developing electrocatalysts that can exhibit high NH selectivity at high current densities is important for their practical applications, but still remains challenging. Here we demonstrate that molecularly dispersed electrocatalysts (MDEs) of metal phthalocyanines on carbon nanotubes can enable rapid and selective NH production from the NORR and NORR. The copper phthalocyanine (CuPc) MDE shows a much lower overpotential requirement for the NORR than the aggregated CuPc sample, delivering a high NH partial current density of ∼1 A cm with a faradaic efficiency (FE) of NH over 98%. Due to the favorable NO absorption, the cobalt phthalocyanine (CoPc) MDE shows higher activity than the CuPc MDE for the NORR, but FE(NH)s of the CoPc MDE at high current densities are limited by its enhanced hydrogen evolution activity. It is further found that the CoPc MDE is more active in the NORR than in the NORR, which is opposite to the CuPc MDE. Thus, the CoPc MDE employed for the NORR can overcome the limitation of the hydrogen evolution reaction, showing a high NH partial current density of 466 mA cm with FE(NH) >97%.

SCI

English

First ; Corresponding

National Natural Science foundation of China[22075125] ; Guangdong-Hong Kong-Macao Joint Laboratory Fund[2019B121205001] ; Shenzhen fundamental research funding[JCYJ20220530114607017]

Chemistry ; Energy & Fuels ; Engineering ; Environmental Sciences & Ecology

Chemistry, Multidisciplinary ; Energy & Fuels ; Engineering, Chemical ; Environmental Sciences

WOS:000971944400001

ROYAL SOC CHEMISTRY

2-s2.0-85153277785

Scopus

1.Department of Materials Science and Engineering,Southern University of Science and Technology,Shenzhen,518055,China
2.Department of Chemistry,Guangdong Provincial Key Laboratory of Catalysis,Southern University of Science and Technology,Shenzhen,China
3.State Key Laboratory of Clean Energy Utilization,State Environmental ProtectionCenter for Coal-Fired Air Pollution Control,Zhejiang University,Hangzhou,310027,China
4.Guangdong-Hong Kong-Macao Joint Laboratory for Photonic-Thermal-Electrical Energy Materials and Devices,Southern University of Science and Technology,Shenzhen,518055,China

Jiang，Zhan,Wang，Yamin,Lin，Zhicao,et al. Molecular electrocatalysts for rapid and selective reduction of nitrogenous waste to ammonia[J]. Energy and Environmental Science,2023,16(5).

Jiang，Zhan.,Wang，Yamin.,Lin，Zhicao.,Yuan，Yubo.,Zhang，Xiao.,...&Liang，Yongye.(2023).Molecular electrocatalysts for rapid and selective reduction of nitrogenous waste to ammonia.Energy and Environmental Science,16(5).

Jiang，Zhan,et al."Molecular electrocatalysts for rapid and selective reduction of nitrogenous waste to ammonia".Energy and Environmental Science 16.5(2023).