In:
Journal of Materials Chemistry A, Royal Society of Chemistry (RSC), Vol. 10, No. 47 ( 2022), p. 25356-25362
Abstract:
The scale-up syntheses of electrocatalysts with rationally designed functional promoter groups that can directly interact with catalytic-centres are much desired for CO 2 electroreduction. Here, we propose an in situ copolymerization method that can be applied for the scale-up syntheses of metalloporphyrin based conjugated porous polymers with directly interacting catalytic centres and promoter groups. The thus-obtained materials possess the characteristics of high porosity, adjustable morphology, abundant catalytic sites and directly interacting promoter groups. In particular, CPP–Cu with ferrocene as the promoter group exhibits a FE CH 4 +C 2 H 4 of 94.0% (FE CH 4 , 75.9%, FE C 2 H 4 , 18.1%, −0.9 V), which is much higher than that of Cu-porphyrin, Bz-CPP-Cu and the physical-mixture and represents one of the best electro-catalysts so far. DFT calculations reveal that the directly-interacting ferrocene groups could enhance the electron-cloud density of Cu-porphyrin and possess strong adsorption-ability to OH* to kinetically improve the proton-coupled electron transfer for the preferential CO 2 -to-CH 4 pathway. Noteworthily, the synthesis-strategy is easy to scale-up (∼10 g in a batch-experiment) and the reaction-time can be as little as 10 min under microwave-conditions.
Type of Medium:
Online Resource
ISSN:
2050-7488
,
2050-7496
Language:
English
Publisher:
Royal Society of Chemistry (RSC)
Publication Date:
2022
detail.hit.zdb_id:
2702232-8
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