It is fascinating to explore the distribution of CO_(2)hydrogenation products regulated by heterogeneous catalysts,as both the chemical state of surface metals and structure of the support itself of the supported cata...It is fascinating to explore the distribution of CO_(2)hydrogenation products regulated by heterogeneous catalysts,as both the chemical state of surface metals and structure of the support itself of the supported catalysts may affect the performance of CO_(2)hydrogenation.Herein,the complete switching of CO_(2)hydrogenation products from CH4 to CO can be realized by induction of Cl into Ru/TiO_(2)catalyst.Density functional theory(DFT)calculations indicated that Cl ions were mainly located on the Ru metal sites of Ru/TiO_(2)catalysts.Bader charge analysis and Ru 3p X-ray photoelectron spectra(XPS)results suggested that electrons transferred from Ru to Cl,resulting in the decrease of electron density of Ru.In situ diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS)of CO_(2)hydrogenation and CO adsorption proved that with the increase of the Cl ion content,the adsorption of CO on the catalyst surface was significantly weakened,and resulted in the high CO selectivity.Our work demonstrates the role of Cl ions in regulating the distribution of CO_(2)hydrogenation products,and provides new ideas for regulating other catalytic processes.展开更多
Lignin,as the second largest renewable biomass resource in nature,has increasingly received significant interest for its potential to be transformed into valuable chemicals,potentially contributing to carbon neutralit...Lignin,as the second largest renewable biomass resource in nature,has increasingly received significant interest for its potential to be transformed into valuable chemicals,potentially contributing to carbon neutrality.Among different approaches,renewable electricity-driven biomass conversion holds great promise to substitute a petroleum resource-driven one,owing to its characteristics of environmental friendliness,high energy efficiency,and tunable reactivity.The challenges lie on the polymeric structure and complex functional groups in lignin,requiring the development of efficient electrocatalysts for lignin valorization with enhanced activity and selectivity toward targeted chemicals.In this Review,we focus on the advancement of electrocatalytic valorization of lignin,from monomers,to dimers and to raw lignin,toward various valueadded chemicals,with emphasis on catalyst design,reaction innovation,and mechanistic study.The general strategies for catalyst design are also summarized,offering insights into enhancing the activity and selectivity.Finally,challenges and perspectives for the electrocatalytic conversion of lignin are proposed.展开更多
基金the National Natural Science Foundation of China(No.22072176)the Key Laboratory of Magnetic Molecules and Magnetic Information Materials,Ministry of Education(No.MMMM-202001)+1 种基金the Shanxi Science and Technology Department(No.20210302123012)the Award Foundation for Excellent PhD Graduates Work in Shanxi Province(No.SQ2019005).
文摘It is fascinating to explore the distribution of CO_(2)hydrogenation products regulated by heterogeneous catalysts,as both the chemical state of surface metals and structure of the support itself of the supported catalysts may affect the performance of CO_(2)hydrogenation.Herein,the complete switching of CO_(2)hydrogenation products from CH4 to CO can be realized by induction of Cl into Ru/TiO_(2)catalyst.Density functional theory(DFT)calculations indicated that Cl ions were mainly located on the Ru metal sites of Ru/TiO_(2)catalysts.Bader charge analysis and Ru 3p X-ray photoelectron spectra(XPS)results suggested that electrons transferred from Ru to Cl,resulting in the decrease of electron density of Ru.In situ diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS)of CO_(2)hydrogenation and CO adsorption proved that with the increase of the Cl ion content,the adsorption of CO on the catalyst surface was significantly weakened,and resulted in the high CO selectivity.Our work demonstrates the role of Cl ions in regulating the distribution of CO_(2)hydrogenation products,and provides new ideas for regulating other catalytic processes.
基金supported by the National Key R&D Program of China(2023YFA1507400)the Haihe Laboratory of Sustainable Chemical Transformations,the National Natural Science Foundation of China(Grant No.22325805,21935001)Beijing Natural Science Foundation(JQ22003).
文摘Lignin,as the second largest renewable biomass resource in nature,has increasingly received significant interest for its potential to be transformed into valuable chemicals,potentially contributing to carbon neutrality.Among different approaches,renewable electricity-driven biomass conversion holds great promise to substitute a petroleum resource-driven one,owing to its characteristics of environmental friendliness,high energy efficiency,and tunable reactivity.The challenges lie on the polymeric structure and complex functional groups in lignin,requiring the development of efficient electrocatalysts for lignin valorization with enhanced activity and selectivity toward targeted chemicals.In this Review,we focus on the advancement of electrocatalytic valorization of lignin,from monomers,to dimers and to raw lignin,toward various valueadded chemicals,with emphasis on catalyst design,reaction innovation,and mechanistic study.The general strategies for catalyst design are also summarized,offering insights into enhancing the activity and selectivity.Finally,challenges and perspectives for the electrocatalytic conversion of lignin are proposed.
