Although Sn-based catalysts have recently achieved considerable improvement in selective electro-catalyzing CO_(2)into HCOOH,the role of various valence Sn species is not fully understood due to the complexity and unc...Although Sn-based catalysts have recently achieved considerable improvement in selective electro-catalyzing CO_(2)into HCOOH,the role of various valence Sn species is not fully understood due to the complexity and uncertainty of their evolution during the reaction process.Here,inspired by the theoretical simulations that the concomitant multivalent Sn(Sn^(0),Sn^(Ⅱ)and Sn^(Ⅳ))can significantly motivate the intrinsic activity of Sn-based catalyst,the Sn/SnO/SnO_(2)nanosheets were proposed to experimentally verify the synergistic effect of multivalent Sn species on the CO_(2)-into-HCOOH conversion.During CO_(2)reduction reaction,the Sn/SnO/SnO_(2)nanosheets,which are prepared by the sequential hydrothermal reaction,calcined crystallization and low-temperature H_(2)treatment,exhibit a high FEHCOOH of 89.6%at-0.9 VRHE as well as a large cathodic current density.Systematic experimental and theoretical results corroborate that multivalent Sn species synergistically energize the CO_(2)activation,the HCOO*adsorption,and the electron transfer,which make Sn/SnO/SnO_(2)favour the conversion from CO_(2)into HCOOH in both thermodynamics and kinetics.This proof-of-concept study establishes a relationship between the enhanced performance and the multivalent Sn species,and also provides a practicable and scalable avenue for rational engineering high-powered electrocatalysts.展开更多
基金the National Natural Science Foundation of China(Nos.21631004,21901065)the Natural Science Foundation of Heilongjiang Province of China(No.LH2020B019)+1 种基金the Youth Science and Technology Innovation Team Project of Heilongjiang Province(No.RCYJTD201803)the University Nursing Program for Young Scholars with Creative Talents in Heilongjiang Province(No.UNPYSCT-2018009).
文摘Although Sn-based catalysts have recently achieved considerable improvement in selective electro-catalyzing CO_(2)into HCOOH,the role of various valence Sn species is not fully understood due to the complexity and uncertainty of their evolution during the reaction process.Here,inspired by the theoretical simulations that the concomitant multivalent Sn(Sn^(0),Sn^(Ⅱ)and Sn^(Ⅳ))can significantly motivate the intrinsic activity of Sn-based catalyst,the Sn/SnO/SnO_(2)nanosheets were proposed to experimentally verify the synergistic effect of multivalent Sn species on the CO_(2)-into-HCOOH conversion.During CO_(2)reduction reaction,the Sn/SnO/SnO_(2)nanosheets,which are prepared by the sequential hydrothermal reaction,calcined crystallization and low-temperature H_(2)treatment,exhibit a high FEHCOOH of 89.6%at-0.9 VRHE as well as a large cathodic current density.Systematic experimental and theoretical results corroborate that multivalent Sn species synergistically energize the CO_(2)activation,the HCOO*adsorption,and the electron transfer,which make Sn/SnO/SnO_(2)favour the conversion from CO_(2)into HCOOH in both thermodynamics and kinetics.This proof-of-concept study establishes a relationship between the enhanced performance and the multivalent Sn species,and also provides a practicable and scalable avenue for rational engineering high-powered electrocatalysts.
