Calcium sulfate(CaSO_(4))has been verified as a promising oxygen carrier(OC)in the chemical looping combustion(CLC)for its high oxygen capacity,abundant reserve and low cost,but its low reactivity and deleterious sulf...Calcium sulfate(CaSO_(4))has been verified as a promising oxygen carrier(OC)in the chemical looping combustion(CLC)for its high oxygen capacity,abundant reserve and low cost,but its low reactivity and deleterious sulfur species emission from the side reactions of CaSO_(4) should be well considered for its wide application in CLC.In order to promote the reactivity of CaSO_(4) and increase its potential to inhibit the gaseous sulfur emission,a CeO_(2)-enhanced CaSO_(4) OC mixed OC of core–shell structure was prepared using the combined template synthesis method.Reaction characteristics of the prepared CaSO_(4)-CeO_(2) mixed OC with a typical lignite was first conducted and systematically investigated,and an improved reactivity of the prepared CaSO_(4)-CeO_(2) mixed OC was demonstrated than its single component CaSO_(4) or CeO_(2) due to the fast transfer and exchange of oxygen from the CaSO_(4) substrate to coal via the doped CeO_(2).Furthermore,the solid products formed from the mixed CaSO_(4)-CeO_(2) OC with the selected coal were collected and analyzed.Especially,evolution and redistribution of the sulfur species of different forms were focused.At the latter reaction stage of YN reaction with the CaSO_(4)-CeO_(2) mixed OC,the SO_(2) emitted from the side reactions of CaSO_(4) was greatly diminished and the doped CeO_(2) was proven effective to directionally fix the SO_(2) released to turn into different solid sulfur compounds,which were determined as Ce_(2)O_(2)S,Ce_(2)S_(3) and Ce_(2)(SO_(4))_(3)·5H_(2)O and formed through the different pathways.In addition,good regeneration of the reduced CaSO_(4)-CeO_(2) mixed OC could be reached in spite of the unavoidable interaction between the included minerals in coal and the reduced mixed OC.Overall,the combined template method-made CaSO_(4)-CeO_(2) mixed OC reported herein was not only endowed with enhanced reactivity for coal conversion,but also owned the potential to directionally fix the gaseous sulfur emission,which is quite applicable as OC for simultaneous decarbonatization and desulfurization in the real CLC process.展开更多
The electrocatalytic sulfur reduction reaction(SRR)and sulfur evolution reaction(SER),two fundamental multistep conversion processes in lithium–sulfur batteries(LSBs),are root-cause solutions to overcome sluggish red...The electrocatalytic sulfur reduction reaction(SRR)and sulfur evolution reaction(SER),two fundamental multistep conversion processes in lithium–sulfur batteries(LSBs),are root-cause solutions to overcome sluggish redox kinetics and the polysulfide shuttling effect.Metal–organic framework(MOF)electrocatalysts have emerged as good platforms for catalyzing SRR and SER,but their catalytic performance is challenged by poor electrical conductivity and limited chemical stability.Functionalized MOFs and their hybrids may be beneficial for stabilizing and improving the desired catalytic properties to achieve high-performance LSBs.This review provides a detailed overview of engineering principles for improving the activity,selectivity,and stability of MOFrelated electrocatalysts via composition modulation and nanostructure design as well as hybrid assembly.It presents and discusses the various advances achieved by using in situ characterization techniques,simulations,and theoretical calculations to reveal the dynamic evolution of MOF-related electrocatalysts,enabling an in-depth understanding of the catalysis mechanism at the molecular/atomic level.Lastly,prospects and possible research directions for MOF-related sulfur electrocatalysts are proposed.展开更多
To meet the ever-increasing energy demands, advanced electrode materials are strongly requested for the exploration of advanced energy storage and conversion technologies, such as Li-ion batteries, Li-S batteries, Li-...To meet the ever-increasing energy demands, advanced electrode materials are strongly requested for the exploration of advanced energy storage and conversion technologies, such as Li-ion batteries, Li-S batteries, Li-]Zn-air batteries, supercapacitors, dye-sensitized solar cells, and other electrocatalysis process (e.g., oxygen reductionlevolution reaction, hydrogen evolution reaction). Transition metal chalcogenides (TMCs, Le., sulfides and selenides) are forcefully considered as an emerging candidate, owing to their unique physical and chemical properties. Moreover, the integration of TMCs with conductive graphene host has enabled the significant improvement of electrochemical performance of devices. In this review, the recent research progress on TMC]graphene composites for applications in energy storage and conversion devices is summarized. The preparation process of TMC]graphene nanocomposites is also included. In order to promote an in-depth understanding of performance improvement for TMC/graphene materials, the operating principle of various devices and technologies are briefly presented. Finally, the perspectives are given on the design and construction of advanced electrode materials.展开更多
基金supported by the National Natural Science Founda-tion of China(Nos.51776073,51906083)Key Research&Develop-ment program of Henan Province(No.162102210233)+1 种基金North China University of Water Resources and Electric Power Innovative Project(Nos.2019XA014,2019XB058)Scientific Research&Development Project of Ji-Yan Energy Science and Technology Research Institute(NKY2020-05).
文摘Calcium sulfate(CaSO_(4))has been verified as a promising oxygen carrier(OC)in the chemical looping combustion(CLC)for its high oxygen capacity,abundant reserve and low cost,but its low reactivity and deleterious sulfur species emission from the side reactions of CaSO_(4) should be well considered for its wide application in CLC.In order to promote the reactivity of CaSO_(4) and increase its potential to inhibit the gaseous sulfur emission,a CeO_(2)-enhanced CaSO_(4) OC mixed OC of core–shell structure was prepared using the combined template synthesis method.Reaction characteristics of the prepared CaSO_(4)-CeO_(2) mixed OC with a typical lignite was first conducted and systematically investigated,and an improved reactivity of the prepared CaSO_(4)-CeO_(2) mixed OC was demonstrated than its single component CaSO_(4) or CeO_(2) due to the fast transfer and exchange of oxygen from the CaSO_(4) substrate to coal via the doped CeO_(2).Furthermore,the solid products formed from the mixed CaSO_(4)-CeO_(2) OC with the selected coal were collected and analyzed.Especially,evolution and redistribution of the sulfur species of different forms were focused.At the latter reaction stage of YN reaction with the CaSO_(4)-CeO_(2) mixed OC,the SO_(2) emitted from the side reactions of CaSO_(4) was greatly diminished and the doped CeO_(2) was proven effective to directionally fix the SO_(2) released to turn into different solid sulfur compounds,which were determined as Ce_(2)O_(2)S,Ce_(2)S_(3) and Ce_(2)(SO_(4))_(3)·5H_(2)O and formed through the different pathways.In addition,good regeneration of the reduced CaSO_(4)-CeO_(2) mixed OC could be reached in spite of the unavoidable interaction between the included minerals in coal and the reduced mixed OC.Overall,the combined template method-made CaSO_(4)-CeO_(2) mixed OC reported herein was not only endowed with enhanced reactivity for coal conversion,but also owned the potential to directionally fix the gaseous sulfur emission,which is quite applicable as OC for simultaneous decarbonatization and desulfurization in the real CLC process.
基金supported by the National Key R&D Program of China(2021YFB3800300)Beijing Outstanding Young Scientists Program(BJJWZYJH01201910007023)Yuanguang Scholars Program,Hebei University of Technology(282022554).
文摘The electrocatalytic sulfur reduction reaction(SRR)and sulfur evolution reaction(SER),two fundamental multistep conversion processes in lithium–sulfur batteries(LSBs),are root-cause solutions to overcome sluggish redox kinetics and the polysulfide shuttling effect.Metal–organic framework(MOF)electrocatalysts have emerged as good platforms for catalyzing SRR and SER,but their catalytic performance is challenged by poor electrical conductivity and limited chemical stability.Functionalized MOFs and their hybrids may be beneficial for stabilizing and improving the desired catalytic properties to achieve high-performance LSBs.This review provides a detailed overview of engineering principles for improving the activity,selectivity,and stability of MOFrelated electrocatalysts via composition modulation and nanostructure design as well as hybrid assembly.It presents and discusses the various advances achieved by using in situ characterization techniques,simulations,and theoretical calculations to reveal the dynamic evolution of MOF-related electrocatalysts,enabling an in-depth understanding of the catalysis mechanism at the molecular/atomic level.Lastly,prospects and possible research directions for MOF-related sulfur electrocatalysts are proposed.
基金supported by the National Key Research and Development Program(Nos.2016YFA0202500,2016YFA0200102)the National Natural Science Foundation of China(No.21676160)China Postdoctoral Science Foundation(No.2017M620049)
文摘To meet the ever-increasing energy demands, advanced electrode materials are strongly requested for the exploration of advanced energy storage and conversion technologies, such as Li-ion batteries, Li-S batteries, Li-]Zn-air batteries, supercapacitors, dye-sensitized solar cells, and other electrocatalysis process (e.g., oxygen reductionlevolution reaction, hydrogen evolution reaction). Transition metal chalcogenides (TMCs, Le., sulfides and selenides) are forcefully considered as an emerging candidate, owing to their unique physical and chemical properties. Moreover, the integration of TMCs with conductive graphene host has enabled the significant improvement of electrochemical performance of devices. In this review, the recent research progress on TMC]graphene composites for applications in energy storage and conversion devices is summarized. The preparation process of TMC]graphene nanocomposites is also included. In order to promote an in-depth understanding of performance improvement for TMC/graphene materials, the operating principle of various devices and technologies are briefly presented. Finally, the perspectives are given on the design and construction of advanced electrode materials.