期刊
SMARTMAT
卷 3, 期 1, 页码 151-162出版社
WILEY
DOI: 10.1002/smm2.1081
关键词
carbon dioxide reduction; cobalt complex; disubstituted quaterpyridine; heterogeneous molecular catalysis; second coordination sphere
资金
- Zhejiang Provincial Natural Science Foundation of China [LZ20B030001]
- Agency for Science, Technology, and Research (A*STAR), Singapore [A1983c0026]
- Campus for Research Excellence and Technological Enterprise (CREATE) program, National Research Foundation (NRF), Prime Minister's Office, Singapore
- National Natural Science Foundation of China [21972106, 51872209]
Researchers have developed a cobalt complex catalyst based on disubstituted quaterpyridine, which is non-covalently tethered to a multiwalled carbon nanotube substrate. This hybrid catalyst, Co-qpyCOOH/CNT, demonstrates remarkable catalytic activity, near-exclusive selectivity, and high stability for the conversion of CO2 to CO under aqueous conditions. With a mere cathodic potential of -0.65 V versus RHE, it achieves a high partial current density of -6.7 mA/cm(2) and a CO selectivity of 100%.
A disubstituted quaterpyridine based cobalt complex non-covalently tethered to multiwalled carbon nanotube (MWCNT) substrate, forming a hybrid catalyst, Co-qpyCOOH/CNT, catalyzed the conversion of CO2 to CO under aqueous conditions. At an optimal and uniform loading, it exhibited remarkable catalytic activity, near-exclusive selectivity, and high stability towards the formation of CO. At a mere cathodic potential of -0.65 V versus RHE (eta = 0.54 V), it achieved a high partial current density of -6.7 mA/cm(2) and a F.E.(CO) = 100%. In addition, with 20 h of stable operation, hydrogen evolution remained practically undetected. Its hybrid structure due to noncovalent immobilization on MWCNT imparted the intrinsic activity and much-needed stability in performance whereas -COOH groups may stabilize the intermediates by acting as H-bond donors, promoting catalytic activity. Tethering to a conductive solid substrate and tuning of the second sphere of coordination played an important role in its performance to achieve desired reduction product with high selectivity and activity.
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