Metastable Phase Cu with Optimized Local Electronic State for Efficient Electrocatalytic Production of Ammonia from Nitrate

Weidong Wen; Ping Yan; Wanping SunYitong ZhouXin-Yao Yu

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Metastable Phase Cu with Optimized Local Electronic State for Efficient Electrocatalytic Production of Ammonia from Nitrate

机译：Metastable Phase Cu with Optimized Local Electronic State for Efficient Electrocatalytic Production of Ammonia from Nitrate

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Electrocatalytic nitrate (NO_3~?) reduction reaction (NITRR) is an inspiringroute for ammonia (NH_3) synthesis at ambient condition. The metallic Cubasedmaterial with low cost and high activity is one of the most promisingelectrocatalysts for NITRR. However, due to the weaker atomic H~*-providingcapacity, the produced intermediate-nitrite tends to accumulate on itssurface, leading to unsatisfactory NH_3 selectivity and Faradic efficiency (FE).Herein, a novel and facile O_2/Ar plasma oxidation and subsequent electroreductionstrategy is developed to synthesize a kind of metastable phase Cu.Excitingly, the metastable phase Cu demonstrates superior NITRR performanceto conventional phase Cu with high NH_4~+ selectivity (97.8) and FE(99.8). Density function theory (DFT) calculations reveal that the upshift ofthe d-band center to near the Fermi level in metastable phase Cu contributesto the enhanced activity, while the relatively strong adsorption of H~* facilitatesthe conversion from NO_2~*/NO~* to NOOH~*/NOH~* and thus ensureshigh selectivity and FE. Furthermore, when evaluated as cathode materialin Zn-NO_3~? battery, high power density (7.56 mW cm~(?2)) and NH_4~+ yield(76 μmol h~(?1) cm~(?2)) are achieved by the metastable phase Cu-based battery.

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来源
《Advanced functional materials》 |2023年第6期|2212236.1-2212236.11|共11页
作者
Weidong Wen; Ping Yan; Wanping SunYitong ZhouXin-Yao Yu;
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作者单位

School of Materials Science and Engineering Anhui University Hefei 230601, P. R. China,Institute of Energy Hefei Comprehensive National Science Center (Anhui Energy Laboratory) Hefei 230001, P. R. China;

School of Materials Science and Engineering Anhui University Hefei 230601, P. R. China;

Institute of Energy Hefei Comprehensive National Science Center (Anhui Energy Laboratory) Hefei 230001, P. R. China,Institutes of Physical Science and Information Technology Anhui University Hefei 230601, P. R. ChinaInstitutes of Physical Science and Information Technology Anhui University Hefei 230601, P. R. China;

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ammonia synthesis; electrocatalysts; metastable phase Cu; nitrate;

Metastable Phase Cu with Optimized Local Electronic State for Efficient Electrocatalytic Production of Ammonia from Nitrate

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