Asymmetric acidic/alkaline N2 electrofixation accelerated by high‐entropy metal–organic framework derivatives
Yuntong Sun,
Wenqiang Wu,
Lei Yu,
Shuaishuai Xu,
Yuxiang Zhang,
Licheng Yu,
Baokai Xia,
Shan Ding,
Ming Li,
LiLi Jiang,
Jingjing Duan,
Junwu Zhu,
Sheng Chen
Affiliations
Yuntong Sun
Key Laboratory for Soft Chemistry and Functional Materials, School of Chemistry and Chemical Engineering, School of Energy and Power Engineering Nanjing University of Science and Technology Nanjing Jiangsu China
Wenqiang Wu
Key Laboratory for Soft Chemistry and Functional Materials, School of Chemistry and Chemical Engineering, School of Energy and Power Engineering Nanjing University of Science and Technology Nanjing Jiangsu China
Lei Yu
Key Laboratory for Soft Chemistry and Functional Materials, School of Chemistry and Chemical Engineering, School of Energy and Power Engineering Nanjing University of Science and Technology Nanjing Jiangsu China
Shuaishuai Xu
Key Laboratory for Soft Chemistry and Functional Materials, School of Chemistry and Chemical Engineering, School of Energy and Power Engineering Nanjing University of Science and Technology Nanjing Jiangsu China
Yuxiang Zhang
Key Laboratory for Soft Chemistry and Functional Materials, School of Chemistry and Chemical Engineering, School of Energy and Power Engineering Nanjing University of Science and Technology Nanjing Jiangsu China
Licheng Yu
Key Laboratory for Soft Chemistry and Functional Materials, School of Chemistry and Chemical Engineering, School of Energy and Power Engineering Nanjing University of Science and Technology Nanjing Jiangsu China
Baokai Xia
Key Laboratory for Soft Chemistry and Functional Materials, School of Chemistry and Chemical Engineering, School of Energy and Power Engineering Nanjing University of Science and Technology Nanjing Jiangsu China
Shan Ding
Key Laboratory for Soft Chemistry and Functional Materials, School of Chemistry and Chemical Engineering, School of Energy and Power Engineering Nanjing University of Science and Technology Nanjing Jiangsu China
Ming Li
Key Laboratory for Soft Chemistry and Functional Materials, School of Chemistry and Chemical Engineering, School of Energy and Power Engineering Nanjing University of Science and Technology Nanjing Jiangsu China
LiLi Jiang
Key Laboratory for Soft Chemistry and Functional Materials, School of Chemistry and Chemical Engineering, School of Energy and Power Engineering Nanjing University of Science and Technology Nanjing Jiangsu China
Jingjing Duan
Key Laboratory for Soft Chemistry and Functional Materials, School of Chemistry and Chemical Engineering, School of Energy and Power Engineering Nanjing University of Science and Technology Nanjing Jiangsu China
Junwu Zhu
Key Laboratory for Soft Chemistry and Functional Materials, School of Chemistry and Chemical Engineering, School of Energy and Power Engineering Nanjing University of Science and Technology Nanjing Jiangsu China
Sheng Chen
Key Laboratory for Soft Chemistry and Functional Materials, School of Chemistry and Chemical Engineering, School of Energy and Power Engineering Nanjing University of Science and Technology Nanjing Jiangsu China
Abstract High‐entropy materials are composed of five or more metal elements with equimolar or near‐equimolar concentrations within one crystal structure, which offer remarkable structural properties for many applications. Despite previously reported entropy‐driven stabilization mechanisms, many high‐entropy materials still tend to decompose to produce a variety of derivatives under operating conditions. In this study, we use transition‐metal (Ni, Co, Ni, Zn, V)‐based high‐entropy metal–organic frameworks (HE‐MOFs) as the precursors to produce different derivatives under acidic/alkaline treatment. We have shown that HE‐MOFs and derivatives have shown favorable kinetics for N2 electrofixation in different pH electrolytes, specifically cathodic nitrogen reduction reaction in acidic media and anodic oxygen evolution reaction in alkaline media. To buffer the pH mismatch, we have further constructed an asymmetric acidic/alkaline device prototype by using bipolar membranes. As expected, the prototype showed remarkable activities, with an NH3 yield rate of 42.76 μg h−1 mg−1, and Faradaic efficiency of 14.75% and energy efficiency of 2.59%, which are 14.4 and 4.4 times larger than those of its symmetric acidic and alkaline counterparts, respectively.
