Electrochemical dechlorination and hydrocarbon valorization by cobalt phthalocyanine with non-proton-coupled redox property

利用具有非质子耦合氧化还原特性的钴酞菁进行电化学脱氯和烃类增值转化

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Abstract

Electrochemical dechlorination provides a sustainable method to treat chlorinated volatile organic compounds polluted water with producing value-added hydrocarbon. However, dechlorination of dichloromethane (CH(2)Cl(2)) generates *CH(3) and *CH(2)Cl intermediates, which are highly unstable due to lack of efficient hyperconjugation from neighboring carbon sites. Herein, we report that cobalt phthalocyanine (CoPc) grafts onto sulfur-doped graphene toward efficient electrocatalysis of CH(2)Cl(2) dechlorination at moderate potentials. It reveals that sulfoxide groups within graphene linked to Co sites by an axial coordination, resulting in an electron donation effect to decrease the barriers of elemental dechlorination step. While in situ electrochemically generates [Co(1+)Pc]⁻ species mediated the electron transfer from Co sites to CH(2)Cl(2). The production rate of CH(4) is significantly enhanced compares to the current level, and an additional case of producing C(2)H(4) and C(2)H(6) is achieved. For potential practical application, the electrochemical dechlorination of a diluted CH(2)Cl(2) solution is validated in an electrofiltration module setup by an efficient flow-through mode.

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