Self-enhanced localized alkalinity at the encapsulated Cu catalyst for superb electrocatalytic nitrate/nitrite reduction to NH 3 in neutral electrolyte

Author:

Shen Zhen1ORCID,Chen Guanghai1,Cheng Xueyi1,Xu Fengfei1ORCID,Huang Hongwen2ORCID,Wang Xizhang1,Yang Lijun1ORCID,Wu Qiang1ORCID,Hu Zheng1ORCID

Affiliation:

1. Key Laboratory of Mesoscopic Chemistry of MOE and Jiangsu Provincial Laboratory for Nanotechnology, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210023, P. R. China.

2. College of Materials Science and Engineering, Hunan University, Changsha, Hunan 410082, P. R. China.

Abstract

The electrocatalytic nitrate/nitrite reduction reaction (eNO x RR) to ammonia (NH 3 ) is thermodynamically more favorable than the eye-catching nitrogen (N 2 ) electroreduction. To date, the high eNO x RR-to-NH 3 activity is limited to strong alkaline electrolytes but cannot be achieved in economic and sustainable neutral/near-neutral electrolytes. Here, we construct a copper (Cu) catalyst encapsulated inside the hydrophilic hierarchical nitrogen-doped carbon nanocages (Cu@hNCNC). During eNO x RR, the hNCNC shell hinders the diffusion of generated OH ions outward, thus creating a self-enhanced local high pH environment around the inside Cu nanoparticles. Consequently, the Cu@hNCNC catalyst exhibits an excellent eNO x RR-to-NH 3 activity in the neutral electrolyte, equivalent to the Cu catalyst immobilized on the outer surface of hNCNC (Cu/hNCNC) in strong alkaline electrolyte, with much better stability for the former. The optimal NH 3 yield rate reaches 4.0 moles per hour per gram with a high Faradaic efficiency of 99.7%. The strong-alkalinity-free advantage facilitates the practicability of Cu@hNCNC catalyst as demonstrated in a coupled plasma-driven N 2 oxidization with eNO x RR-to-NH 3 .

Publisher

American Association for the Advancement of Science (AAAS)

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