reported a phenomenon that partially oxidized atomic cobalt layers effectively adjusted the electronic structure, promoted the activation of CO 2, and stabilized the relevant key intermediates, thereby enhancing the efficiency of the CO 2 electroreduction to liquid fuel. Previous theoretical calculations have confirmed that the *OCHO binding energy is closely associated with the oxophilicity of the catalyst surface, which can be achieved by modifying the surface of the electrocatalyst with oxygen atom. developed a general amino acid modification approach on Cu electrodes for the selective electroreduction of CO 2 toward hydrocarbons. The surface chemistry modification, as a powerful strategy, has attracted great interest in adjusting electronic properties of active sites to target intermediate adsorption energy as well as harvest high selectivity. Given that the CO 2 molecule activation is closely related to the number and inherent activity of active sites, many effective strategies have been employed to tailor the active sites of electrocatalysts for enhancing the efficiency of the CO 2 electroreduction to formate. To this end, it is of great significance to develop an efficient and durable Sn-based catalysts for the CO 2 electroreduction to formate.

Unfortunately, the catalytic performance of most Sn-based materials is still limited by the high energy barrier for CO 2 activation, which is usually attributed to the poor stabilization of CO 2* − intermediates. Among these electrocatalysts, Sn-based materials have attracted considerable attention due to their advantages of earth abundance, non-toxicity, and low cost. Up to now, various metal-based electrocatalysts, such as Pd, In, Hg, Pb, Cd, and Sn, have been exploited to achieve the CO 2 electroreduction to formate. According to the gross-margin model, formate is considered to be one of the most economically feasible products in the CO 2RR, which can be widely used as an important raw material in the chemical and pharmaceutical industries, as well as a potential hydrogen carrier and the liquid fuel for proton-exchange membrane fuel cell. This result demonstrates the potential strategy of surface oxygen injection for the rational design of advanced catalysts for CO 2 electroreduction.Įlectroreduction of carbon dioxide (CO 2RR) into high-value fuels and feedstocks offers a compelling pathway not only to meet the increasing energy demand, but also to alleviate the environmental crisis caused by CO 2 emissions. Operando synchrotron radiation infrared spectroscopy along with theoretical calculations further reveals that the surface oxygen doping facilitated the CO 2 activation and enhanced the affinity for HCOO* species.

By operando X-ray absorption spectroscopy, we unravel the in situ surface oxygen doping into the matrix during reaction, thereby optimizing the Sn local electronic states. The oxygen-injection SnS 2 nanosheets exhibit a remarkable Faradaic efficiency of 91.6% for carbonaceous products with a current density of 24.1 mA cm −2 at −0.9 V vs RHE, including 83.2% for formate production and 16.5% for syngas with the CO/H 2 ratio of 1:1. Herein, we designed a surface oxygen-injection strategy to tune the electronic structure of SnS 2 nanosheets, which showed effectively enhanced electrocatalytic activity and selectivity of CO 2 reduction to formate and syngas (CO and H 2). Mail.Verifier.4.01.can.end up .right here.We. chemistry modification represents a promising strategy to tailor the adsorption and activation of reaction intermediates for enhancing activity. Thére.is certainly.no. use of. be.sophisticated. usually.a.levels.of.verification.to.

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