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Photoelectrochemical Dicarboxylation of Styrene with CO2 to Phenylsuccinic Acid on Ni-Decorated Silicon Photocathode
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DOI：10.1039/D5GC03730A.png)
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Abstract
En 中文
The conversion of CO2 into value-added chemicals is highly critical for sustainable development. Among the various strategies; the dicarboxylation of alkenes with CO2 offers a highly attractive route to access synthetically valuable dicarboxylic acids; which serve as key intermediates in the production of polymers and pharmaceuticals. Photoelectrochemical (PEC) catalysis carboxylation represents an efficient and sustainable carboxylation strategy; offering distinct advantages including mild reaction conditions; cost-effectiveness; and environmental compatibility. In this study; an efficient PEC system is presented for the carboxylation of styrene using a Ni-modified p-type micro-pyramid silicon (Ni/p-Si) photocathode. The incorporation of Ni catalyst significantly suppresses charge recombination and accelerates charge transfer at the electrode-electrolyte interface; thereby enhancing the overall photoelectrochemical performance. The optimized Ni/p-Si photocathode achieved 77.7% Faradaic efficiency (FE) for phenylsuccinic acid at −2.4 V vs. Ag/AgCl; with a photocurrent density of −4.5 mA cm−2. Moreover; this PEC platform demonstrates moderate FEs across a range of substituted styrenes; indicating good functional group tolerance. Mechanistic studies reveal that the reaction proceeds via single-electron reduction of styrene to generate radical anions; which undergo CO2 addition followed by further reduction and subsequent attack on a second CO2 molecule to yield succinic acid. These findings broaden the scope of CO2 utilization through selective and sustainable C-C bond formation processes.
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9.2
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1.3W
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