Ammonia recovery from nitrate-rich wastewater using a membrane-free electrochemical system

Zhang, Gong; Li, Binggong; Shi, Yanfeng; Zhou, Qi; Fu, Wen-Jie; Zhou, Gang; Ma, Jun; Yin, Shuo; Yuan, Weihao; Miao, Shiyu; Ji, Qinghua; Qu, Jiuhui; Liu, Huijuan

doi:10.1038/s41893-024-01406-7

Nat Sustain

2024

DOI: 10.1038/s41893-024-01406-7

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Ammonia recovery from nitrate-rich wastewater using a membrane-free electrochemical system

Gong Zhang,

Binggong Li,

Yanfeng Shi

et al.

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Conversion of Nitrate to Ammonia by Amidinothiourea-Coordinated Metal Molecular Electrocatalysts with d−π Conjugation

Liu,

Zhao,

et al. 2024

ACS Appl. Mater. Interfaces

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The electrochemical reduction of nitrate to ammonia (NO 3 RR) provides a desired alternative of the traditional Haber−Bosch route for ammonia production, igniting a research boom in the development of electrocatalysts with high activity. Among them, molecular electrocatalysts hold considerable promise for the NO 3 RR, suppressing the competing hydrogen evolution reaction. However, the complicated synthesis procedure, usage of environmentally unfriendly organic solvents, and poor stability of Cu-based molecular electrocatalysts greatly limit their employment in NO 3 RR, and the development of desired Cu-based molecular catalysts remains challenging. Herein, a simple nonorganic solvent involving a one-step strategy was proposed to synthesize d−πconjugated molecular electrocatalysts metal−amidinothiourea (M-ATU). Cu-ATU is composed of Cu coordinated with two S and two N atoms, whereas Ni-ATU is formed by Ni with four N atoms from two ATU ligands. Remarkably, Cu-ATU with a Cu−N 2 S 2 coordination configuration exhibits superior NO 3 RR activity with a NH 3 yield rate of 159.8 mg h −1 mg cat −1 (−1.54 V) and Faradaic efficiency of 91.7% (−1.34 V), outperforming previously reported molecular catalysts. Compared to Ni-ATU, Cu-ATU transfers more electrons to the *NO intermediate, effectively breaking the strong sp 2 hybridization system and weakening the energy of N� O bonds. The increase in free energy of *NO reduced the energy barriers of the rate-determining step, facilitating the further hydrogenation process over Cu-ATU. Our work opened up a new horizon for exploring molecular electrocatalysts for nitrate activation and paved a way for the in-depth understanding of catalytic behaviors, aligning more closely with industrial demands.

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Conversion of Nitrate to Ammonia by Amidinothiourea-Coordinated Metal Molecular Electrocatalysts with d−π Conjugation

Liu,

Zhao,

et al. 2024

ACS Appl. Mater. Interfaces

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En route to a circular nitrogen economy

Shi,

Zhu

2024

Nat Sustain

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Ammonia recovery from nitrate-rich wastewater using a membrane-free electrochemical system

Cited by 2 publications

References 50 publications

Conversion of Nitrate to Ammonia by Amidinothiourea-Coordinated Metal Molecular Electrocatalysts with d−π Conjugation

Conversion of Nitrate to Ammonia by Amidinothiourea-Coordinated Metal Molecular Electrocatalysts with d−π Conjugation

En route to a circular nitrogen economy

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