4.8 Article

Self-Assembly of Hydroxyl Metal-Organic Polyhedra and Polymer into Cu-Based Hollow Spheres for Product-Selective CO2 Electroreduction

期刊

SMALL STRUCTURES
卷 2, 期 7, 页码 -

出版社

WILEY
DOI: 10.1002/sstr.202100012

关键词

calcium carbonate; CO2 electroreduction; hollow spheres; metal-organic polyhedra; polymers

资金

  1. NSFC [21871141, 21871142, 21701085, 21901122]
  2. NSF of Jiangsu Province of China [BK20171032]
  3. Natural Science Research of Jiangsu Higher Education Institutions of China [17KJB150025, 19KJB150011]
  4. China Postdoctoral Science Foundation [2018M630572, 2019M651873]
  5. Priority Academic Program Development of Jiangsu Higher Education Institutions
  6. Foundation of Jiangsu Collaborative Innovation Center of Biomedical Functional Materials

向作者/读者索取更多资源

This research addresses the challenges in selective production of target products in CO2RR by synthesizing Cu-based hollow spheres, allowing for precise generation of various products. The introduction of CaCO3 enables effective tuning of products from C2H4 to CH4, increasing hydrocarbon selectivity and CO2 reduction efficiency.
The electrochemical CO2 reduction reaction (CO2RR), an elegant solution to mitigate the greenhouse effect and produce high-value feedstock, has significant hurdles in selective production of target products. Herein, a series of Cu-based hollow spheres is synthesized through the self-assembly of hydroxyl metal-organic polyhedra and a polymer. The obtained materials with tunable morphology and compositions enable precise generation of varied products in a flow cell. Specifically, polymer-induced sol-gel (PISG)-3 shows 61.1% (-0.9 V, -143 mA cm(-2)) Faradaic efficiency (FE) of C2H4 and negligible CH4, higher than that of PISG-1 (FEC2H4 46.7%) with solid-sphere morphology. Interestingly, the products can be well tuned from C2H4 to CH4 by introducing CaCO3, along with increased hydrocarbon selectivity and CO2 reduction efficiency. Notably, PISG-8 with modified composition displays drastically changed products (FECH4 55.8% and FEC2H4 22.2%, -162 mA cm(-2), -0.9 V). As certified by density functional theory calculations, CaCO3 is proven to decrease the possibility for coexistence of two adjacent *CHO to restrain the dimerization process and enhance the CH4 selectivity.

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