Effective boosting of halogenated α, β-unsaturated C4-dicarbonyl electrocatalytic hydrodehalogenation by 1 T′-MoS2/Ti3C2T2 (T = O, OH, F) heterojunctions: A theoretical study

Halogenated α, β-unsaturated C4-dicarbonyl (X-BDA), a novel family of high-toxicity ring cleavage products, is produced during the disinfection of phenolic compounds. The technique of electrocatalytic hydrodehalogenation (ECH) is efficient in rupturing carbon-halogen bonds and generating useful chemicals. This study used first principles to examine the ECH reaction mechanism of X-BDA and the subsequent hydrogenation reaction of the toxic derivative BDA over the 1 T'-MoS2/Ti3C2T2 (T = O, OH, F) catalysts. The catalytic activity of Ti3C2T2 (T = O, OH, F) catalysts decreases gradually with -OH, -F, -O functional group. The loading of 1 T'-MoS2 onto the Ti3C2T2 surface improves the stability and selectivity of Ti3C2T2. In particular, 1 T'-MoS2/Ti3C2(OH)2 is most conducive to the ECH reaction of X-BDA via a direct-indirect continuous reduction process. It exhibits excellent removal capability towards Cl-BDA, with decreasing reactivity in the order of the Cl-, Br-, and I-BDA. The material offers a solution to the challenging dechlorination issue. The dehalogenated product BDA can be hydrogenated to produce 1,4-butanedial, 1,4-butanediol, and 1,4-butenediol. Three valuable chemicals can be obtained by exerting an applied potential of - 0.65 V. This work suggests that the formation of heterojunction catalyst may lead to new strategies to improve ECH for environmental remediation applications.