Hydrogen has attracted widespread attention as a carbon-neutral energy source,but developing efficient and safe hydrogen storage technologies remains a huge challenge.Recently,liquid organic hydrogen carriers(LOHCs)te...Hydrogen has attracted widespread attention as a carbon-neutral energy source,but developing efficient and safe hydrogen storage technologies remains a huge challenge.Recently,liquid organic hydrogen carriers(LOHCs)technology has shown great potential for efficient and stable hydrogen storage and transport.This technology allows for safe and economical large-scale transoceanic transportation and long-cycle hydrogen storage.In particular,traditional organic hydrogen storage liquids are derived from nonrenewable fossil fuels through costly refining procedures,resulting in unavoidable environmental contamination.Biomass holds great promise for the preparation of LOHCs due to its unique carbon-balance properties and feasibility to manufacture aromatic and nitrogen-doped compounds.According to recent studies,almost 100%conversion and 92% yield of benzene could be obtained through advanced biomass conversion technologies,showing great potential in preparing biomass-based LOHCs.Overall,the present LOHCs systems and their unique applications are introduced in this review,and the technical paths are summarized.Furthermore,this paper provides an outlook on the future development of LOHCs technology,focusing on biomass-derived aromatic and N-doped compounds and their applications in hydrogen storage.展开更多
N-Ethylcarbazole(NEC)is one of the most promising liquid organic hydrogen carriers(LOHCs),but its application is limited by sluggish kinetics due to lack of high-efficiency,low-cost catalysts.This work reports a cobal...N-Ethylcarbazole(NEC)is one of the most promising liquid organic hydrogen carriers(LOHCs),but its application is limited by sluggish kinetics due to lack of high-efficiency,low-cost catalysts.This work reports a cobalt(Co)-based catalyst promoted by nonstoichiometric yttrium hydride(YH_(3−x))to achieve high-efficiency,reversible hydrogen storage in NEC,with>5.5 wt%reversible hydrogen storage capacity could be achieved below 473 K,and with good kinetics.The YH_(3−x)-promoted Co-based catalyst is the first non-noble metal catalyst with high activity for NEC hydrogenation and 12H-NEC dehydrogenation reactions.A mechanistic study suggests that YH_(3−x)facilitates the reversible hydrogen transfer both in the hydrogenation and the dehydrogenation reactions.The nonstoichiometric YH_(3−x)contained both lattice H and H vacancies with tunable H chemical potential serve as the H donor and H acceptor for reversible hydrogen transfer.Our results support the practical application of LOHCs and inspire new approaches for the utilization of conventional metal hydrides to promote versatile H transfer reactions.展开更多
Hydrogen storage in Liquid Organic Hydrogen Carrier(LOHC)systems is appealing for the safe storage and distribution of excess renewable energy via existing gasoline infrastructures to end-users.We present the eutectic...Hydrogen storage in Liquid Organic Hydrogen Carrier(LOHC)systems is appealing for the safe storage and distribution of excess renewable energy via existing gasoline infrastructures to end-users.We present the eutectic mixture of biphenyl and diphenyl ether of its first use as a LOHC material.The material is hydrogenated with 99%selectivity without the cleavage of C–O bond,with commercial heterogeneous catalysts,which is confirmed by nuclear magnetic spectroscopy and gas chromatography-mass spectrometry.Equilibrium concentration,dehydrogenation enthalpy,and thermo-neutral temperature are calculated using a density functional theory.The results indicate that O-atom-containing material exhibits more favorable dehydrogenation thermodynamics than that of the hydrocarbon analogue.The H2-rich material contains6.8 wt%of gravimetric hydrogen storage capacity.A preliminary study of catalytic dehydrogenation on a continuous reactor is presented to demonstrate a reversibility of this material.展开更多
利用电化学、电学等手段研究利用浸渍-还原技术在Nafion膜上制备Au电极的方法,考查Au络合物浸渍时间、还原剂浓度、还原温度等因素对Au/Nafion电极性能的影响。研究发现:较长的浸渍时间、较低的还原剂浓度和较高的还原温度下所制备的电...利用电化学、电学等手段研究利用浸渍-还原技术在Nafion膜上制备Au电极的方法,考查Au络合物浸渍时间、还原剂浓度、还原温度等因素对Au/Nafion电极性能的影响。研究发现:较长的浸渍时间、较低的还原剂浓度和较高的还原温度下所制备的电极活性较好,同时以Na2SO3作为还原剂时,可得到表面Au颗粒均匀堆积的Au/Nafion复合电极。对比利用浸渍-还原技术制备的Pt/Nafion电极和浸渍-还原法制备的Au/Nafion电极在水-苯体系电化学加氢反应中的电极活性。结果表明:苯在阴极的加氢反应主要产物为环己烯和环己烷,且在高阴极过电势下主要生成环己烷;利用Au/Nafion电极实现苯在阴极的加氢还原反应总电流效率可达40%~90%(-1.6^-0.4V vs SCE),析氢副反应在Au/Nafion电极上得到较好抑制。展开更多
基金supported by the National Natural Science Fund for Excellent Young Scholars(China)(Grant No.51822604).
文摘Hydrogen has attracted widespread attention as a carbon-neutral energy source,but developing efficient and safe hydrogen storage technologies remains a huge challenge.Recently,liquid organic hydrogen carriers(LOHCs)technology has shown great potential for efficient and stable hydrogen storage and transport.This technology allows for safe and economical large-scale transoceanic transportation and long-cycle hydrogen storage.In particular,traditional organic hydrogen storage liquids are derived from nonrenewable fossil fuels through costly refining procedures,resulting in unavoidable environmental contamination.Biomass holds great promise for the preparation of LOHCs due to its unique carbon-balance properties and feasibility to manufacture aromatic and nitrogen-doped compounds.According to recent studies,almost 100%conversion and 92% yield of benzene could be obtained through advanced biomass conversion technologies,showing great potential in preparing biomass-based LOHCs.Overall,the present LOHCs systems and their unique applications are introduced in this review,and the technical paths are summarized.Furthermore,this paper provides an outlook on the future development of LOHCs technology,focusing on biomass-derived aromatic and N-doped compounds and their applications in hydrogen storage.
基金This research was made possible as a result of a generous grant from MOST of China(no.2018YFB1502102)NSFC(nos.21771006,51771002,and 51971004).
文摘N-Ethylcarbazole(NEC)is one of the most promising liquid organic hydrogen carriers(LOHCs),but its application is limited by sluggish kinetics due to lack of high-efficiency,low-cost catalysts.This work reports a cobalt(Co)-based catalyst promoted by nonstoichiometric yttrium hydride(YH_(3−x))to achieve high-efficiency,reversible hydrogen storage in NEC,with>5.5 wt%reversible hydrogen storage capacity could be achieved below 473 K,and with good kinetics.The YH_(3−x)-promoted Co-based catalyst is the first non-noble metal catalyst with high activity for NEC hydrogenation and 12H-NEC dehydrogenation reactions.A mechanistic study suggests that YH_(3−x)facilitates the reversible hydrogen transfer both in the hydrogenation and the dehydrogenation reactions.The nonstoichiometric YH_(3−x)contained both lattice H and H vacancies with tunable H chemical potential serve as the H donor and H acceptor for reversible hydrogen transfer.Our results support the practical application of LOHCs and inspire new approaches for the utilization of conventional metal hydrides to promote versatile H transfer reactions.
基金supported by the Technology Development Program to Solve Climate Changes of the National Research Foundation(NRF)funded by the Ministry of Science,ICT,and Future Planning(2015M1A2A2074688)KISTI-HPC(KSC-2018-CRE-0022)for computational resourcesthe KIST institutional program funded by the Korea Institute of Science and Technology(2E29610).
文摘Hydrogen storage in Liquid Organic Hydrogen Carrier(LOHC)systems is appealing for the safe storage and distribution of excess renewable energy via existing gasoline infrastructures to end-users.We present the eutectic mixture of biphenyl and diphenyl ether of its first use as a LOHC material.The material is hydrogenated with 99%selectivity without the cleavage of C–O bond,with commercial heterogeneous catalysts,which is confirmed by nuclear magnetic spectroscopy and gas chromatography-mass spectrometry.Equilibrium concentration,dehydrogenation enthalpy,and thermo-neutral temperature are calculated using a density functional theory.The results indicate that O-atom-containing material exhibits more favorable dehydrogenation thermodynamics than that of the hydrocarbon analogue.The H2-rich material contains6.8 wt%of gravimetric hydrogen storage capacity.A preliminary study of catalytic dehydrogenation on a continuous reactor is presented to demonstrate a reversibility of this material.
文摘利用电化学、电学等手段研究利用浸渍-还原技术在Nafion膜上制备Au电极的方法,考查Au络合物浸渍时间、还原剂浓度、还原温度等因素对Au/Nafion电极性能的影响。研究发现:较长的浸渍时间、较低的还原剂浓度和较高的还原温度下所制备的电极活性较好,同时以Na2SO3作为还原剂时,可得到表面Au颗粒均匀堆积的Au/Nafion复合电极。对比利用浸渍-还原技术制备的Pt/Nafion电极和浸渍-还原法制备的Au/Nafion电极在水-苯体系电化学加氢反应中的电极活性。结果表明:苯在阴极的加氢反应主要产物为环己烯和环己烷,且在高阴极过电势下主要生成环己烷;利用Au/Nafion电极实现苯在阴极的加氢还原反应总电流效率可达40%~90%(-1.6^-0.4V vs SCE),析氢副反应在Au/Nafion电极上得到较好抑制。
