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Tuning d‐Band Structure of CuII in Coordinated Polymer via d–π Conjugation for Improving CO2 Electroreduction Selectivity toward C2 Products

Von Wiley-VCH zur Verfügung gestellt

CO2 reduction: Tuning the d-band structure of CuII center via tetraminobenzoquinone (TABQ) linker with C=O groups regulates the binding energy of electrocatalytic CO2 reduction reaction (CO2RR) intermediates on the catalyst and significantly improves the selectivity towards C2 products, resulting in the highest C2 faradaic efficiency (63.2 %) for CO2RR among metal-coordinated or single-atom catalysts.


Abstract

Copper-coordinated catalysts are reported to be effective for electrocatalytic CO2 reduction reaction (CO2RR) to C2 products but suffer from low selectivity. Herein a strategy was developed to tune the d-band structure of CuII via coordinating with aromatic ligands to form Cu-based conjugated polymers for CO2RR to C2 chemicals. The catalysts derived from copper chloride coordinating with tetraminobenzoquinone (TABQ) and with 1,2,4,5-benzenetetramine possessed high-density and compact Cu single-atom sites and displayed high activity for CO2RR to C2 products. Especially, Cu-TABQ exhibited a maximum C2 faradaic efficiency of 63.2 % with a current density of 423 mA cm−2 at −1.17 V (vs. reversible hydrogen electrode). Density functional theory calculations indicated that the TABQ linker possessing C=O groups significantly widened the d-band of coordinated CuII, which facilitated binding of *CO intermediate on the catalyst and thus enhanced C−C coupling. This work provides mechanistic insight into the CuII-coordinated polymers for CO2RR with high selectivity toward C2 products.

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