Formic acid(FA),which is obtainable through CO_(2)hydrogenation with green hydrogen or biomass conversion,has been used as a prospective liquid organic hydrogen carrier(LOHC)because of the abundant advantages of renew...Formic acid(FA),which is obtainable through CO_(2)hydrogenation with green hydrogen or biomass conversion,has been used as a prospective liquid organic hydrogen carrier(LOHC)because of the abundant advantages of renewability,wide availability,stability,and high volumetric capacity(53 g H_(2)/L).The development of highly efficient catalytic systems to achieve enhanced catalytic activity is attractive but still challenging.Herein,ultrafine and highly dispersed PdAu nanoclusters(NCs)anchored on amino-modified reduced graphene oxide(ArGO)were successfully synthesized via a facile impregnation-reduction method and applied as a catalyst toward formic acid dehydrogenation(FAD).Benefiting from the promoting effect of amino groups,the strain and ligand effect in the alloy,and the Mott–Schottky effect between PdAu NCs and ArGO,the resultant PdAu/ArGO affords an ultrahigh activity under visible light irradiation with an exceptional turnover frequency value of 10,699.5 h^(-1)at 298 K without any additives,more than 2.6times improvement than that under dark,which is the highest among all reported catalysts under the same conditions.This study provides a green and convenient strategy for developing more efficient and sustainable FAD catalysts and promotes the effective utilization of FA as a prospective renewable LOHC.展开更多
Hydrogen,as a clean and efficient energy source,is one of the important energy carriers in the future.However,the safe storage and delivery of hydrogen is still a bottleneck in its practical applications.Chemical hydr...Hydrogen,as a clean and efficient energy source,is one of the important energy carriers in the future.However,the safe storage and delivery of hydrogen is still a bottleneck in its practical applications.Chemical hydrides(such as NaBH_(4),NH_(3)BH_(3),N_(2)H_(4)·H_(2)O,N_(2)H_(4)BH_(3),and HCOOH)are considered as potential chemical hydrogen storage materials that can achieve rapid on-site hydrogen production.At present,the most critical issue for them is to develop economic catalysts to achieve efficient hydrogen production from chemical hydrides.Cop-per(Cu)is considered as a promising catalyst that is one of the most reactive metals among the first-row transition metals and economically cheap.In this review,we outline the recent advancements of Cu-based catalysts in catalyzing hydrogen production from chemical hydrides.Moreover,the synthesis methods,characterization techniques,and hydrogen production catalytic activity of Cu-based catalysts were also introduced.Finally,a brief conclusion and outlook are given for the application of Cu-based catalysts in the dehydrogenation of chemical hydrides.We hope that this review will stimulate interest in the promising research area of Cu-based catalysts for the dehydrogenation of chem-ical hydrides.展开更多
The catalytic performance is highly related to the catalyst structure.Herein,a series of Ni nanoparticles supported on Y_(2)O_(3) with different morphologies were successfully synthesized via hydrothermal process scre...The catalytic performance is highly related to the catalyst structure.Herein,a series of Ni nanoparticles supported on Y_(2)O_(3) with different morphologies were successfully synthesized via hydrothermal process screening different pH environments.These Ni/Y_(2)O_(3)catalysts were applied to efficiently produce CO_(x)-free H2through ammonia decomposition.We identify a significant impact of Y_(2)O_(3)supports on nickel nanoclusters sizes and dispersion.The experimental results show that Ni/Y11 catalyst achieves 100% ammonia decomposition conversion under a gas hour space velocity(GHSV) of 12,000 ml·h^(-1)·gcat^(-1) and temperature of 650℃.Such a high level of activity over Ni/Y11 catalyst was attributed to a large specific surface area,appropriate alkalinity,and small Ni nanoparticles diameter with high dispersion.展开更多
Developing efficient and highly selective catalyst to promote hydrogen generation from hydrous hydrazine(N_(2)H_(4)·H_(2)O) and hydrazine borane(N_(2)H_(4)BH_(3))remains a challenging issue for fuel cell-based hy...Developing efficient and highly selective catalyst to promote hydrogen generation from hydrous hydrazine(N_(2)H_(4)·H_(2)O) and hydrazine borane(N_(2)H_(4)BH_(3))remains a challenging issue for fuel cell-based hydrogen economy.In this work,ultrafine and well-dispersed bimetallic NiPt nanoparticles(3.4 nm) were successfully immobilized on Y_(2)O_(3)-functionalized graphene(Y_(2)O_(3)/rGO) without any surfactant by a simple liquid impregnation approach.It is firstly found that integration of graphene and Y_(2)O_(3) not only can facilitate the formation of ultrafine NiPt nanoparticles(NPs),but also can effectively modulate the electronic structure of NiPt NPs,thereby boosting the catalytic performance.Compared with NiPt/Y_(2)O_(3) and NiPt/rGO,the NiPt/Y_(2)O_(3)/rGO nanocomposites(NCs) show remarkable enhanced catalytic efficiency for hydrogen production from N_(2)H_(4)-H_(2)O.In particular,the optimized Ni_(0.6)Pt_(0.4/)Y_(2)O_(3)/rGO NCs display the best catalytic efficiency and 100% H_(2) selectivity for N_(2)H_(4)-H_(2)O dehydrogenation,providing a turnover frequency(TOF) of2182 h^(-1) at 323 K,which is among the highest values ever reported.Moreover,the Ni_(0.6)Pt_(0.4)/Y_(2)O_(3)/rGO NCs also exhibit an excellent catalytic performance(TOF=3191 h^(-1)) and 100% H_(2) selectively for N_(2)H_(4)BH_(3)dehydrogenation at 323 K.The outstanding catalytic results obtained provide more possibilities for the potential applications of N_(2)H_(4)·H_(2)O and N_(2)H_(4)BH_(3) as promising chemical hydrogen storage materials.展开更多
Development of low-cost and high-performance catalysts for hydrogen generation via hydrolysis of ammonia borane （NH3BH3, AB） is a highly desirable pathway for future hydrogen utilization. In this work, Ni nanocataly...Development of low-cost and high-performance catalysts for hydrogen generation via hydrolysis of ammonia borane （NH3BH3, AB） is a highly desirable pathway for future hydrogen utilization. In this work, Ni nanocatalysts doped with CeOx and supported on graphene （Ni-CeOdgraphene） were synthesized via a facile chemical reduction route and applied as robust catalysts for the hydrolysis of AB in aqueous solution at room temperature. The as-synthesized Ni-CeOdgraphene nanocomposites （NCs） exhibited excellent catalytic activity with a turnover frequency （TOF） as high as 68.2 min-1, which is 49-fold higher than that for a simple Ni nanoparticle catalyst and is among the highest values reported for non-noble metal catalysts in AB hydrolysis. The development of efficient and low-cost Ni-CeOdgraphene catalysts enhances the feasibility of using ammonia borane as a chemical hydrogen storage material, which may find application in a hydrogen fuel-cell based economy.展开更多
Hydrogen has been always the hot topic,which drives a lot of researchers to study and explore hydrogenrelated projects and fields.The first subfield is hydrogen production with green and cost-effective means.Some meth...Hydrogen has been always the hot topic,which drives a lot of researchers to study and explore hydrogenrelated projects and fields.The first subfield is hydrogen production with green and cost-effective means.Some methods have been intensively used for high-efficient hydrogen production,i.e.,catalytic chemical hydrogen generation,electrocatalytic hydrogen evolution,photocatalytic hydrogen evolution,photo-electrocatalytic hydrogen evolution.Most of them are driven by various catalysts.Moreover,the hydrogen storage is also an important question,which is also a present research hot topic,although the history is long with several decades.Hydrogen fuel cells have also obtained great attention due to the zero emissions.The related research mainly focuses on the cell systems and electrocatalysts used.Under this background,we invite some excellent research groups to write this progress on hydrogen from production to utilizations.Finally,we believe that this roadmap on hydrogen can give some useful guidance in future research.展开更多
Formic acid (FA), which can be produced via CO_(2) reduction and biomass conversion, has received extensive interest as a convenient and safe hydrogen carrier due to its wide range of sources, renewable, high hydrogen...Formic acid (FA), which can be produced via CO_(2) reduction and biomass conversion, has received extensive interest as a convenient and safe hydrogen carrier due to its wide range of sources, renewable, high hydrogen content (4.4 wt%), and convenient storage/transportation. Designing highly efficient catalysts is the main challenge to realize the hydrogen production from FA. In this work, well-dispersed and electron-rich PdIr alloy nanoparticles with a size of 1.8 nm are confined in amino-modified 3D mesoporous silica KIT-6 and applied as a highly efficient catalyst for robust hydrogen production from FA at ambient temperature. Small PdIr alloy nanoparticles confined by amino-modified KIT-6 (PdIr/KIT-6-NH_(2)) lead to better catalytic activity compared to that of Pd/KIT-6-NH_(2) and PdIr confined by bare KIT-6, achieving a high turnover frequency (TOF) value of 3533 h-1 at ambient temperature (303 K), 100% H_(2) selectivity and conversion toward the dehydrogenation of FA, which is comparable to the best heterogeneous catalysts ever reported. The high catalytic activity of PdIr/KIT-6-NH_(2) can be attributed to the synergistic effect between Pd and Ir, strong interaction between PdIr and KIT-6-NH_(2), as well as the amino-groups of KIT-6-NH_(2) which can act as a proton scavenger to promote the breaking of O-H bond of formic acid.展开更多
基金financially supported by the National Natural Science Foundation of China(Nos.22162014 and 22162013)Department of Science and Technology of Jiangxi Province(Nos.20212ACB204009,20212BCJL23059 and 20232ACB214002)。
文摘Formic acid(FA),which is obtainable through CO_(2)hydrogenation with green hydrogen or biomass conversion,has been used as a prospective liquid organic hydrogen carrier(LOHC)because of the abundant advantages of renewability,wide availability,stability,and high volumetric capacity(53 g H_(2)/L).The development of highly efficient catalytic systems to achieve enhanced catalytic activity is attractive but still challenging.Herein,ultrafine and highly dispersed PdAu nanoclusters(NCs)anchored on amino-modified reduced graphene oxide(ArGO)were successfully synthesized via a facile impregnation-reduction method and applied as a catalyst toward formic acid dehydrogenation(FAD).Benefiting from the promoting effect of amino groups,the strain and ligand effect in the alloy,and the Mott–Schottky effect between PdAu NCs and ArGO,the resultant PdAu/ArGO affords an ultrahigh activity under visible light irradiation with an exceptional turnover frequency value of 10,699.5 h^(-1)at 298 K without any additives,more than 2.6times improvement than that under dark,which is the highest among all reported catalysts under the same conditions.This study provides a green and convenient strategy for developing more efficient and sustainable FAD catalysts and promotes the effective utilization of FA as a prospective renewable LOHC.
基金supported by the National Natural Science Foundation of China(22162014 and 22162013)Jiangxi Provincial Natural Science Foundation(20232ACB214002)Sponsored Program for Academic and Technical Leaders of Major Disciplines of Jiangxi Province(20212BCJL23059).
文摘Hydrogen,as a clean and efficient energy source,is one of the important energy carriers in the future.However,the safe storage and delivery of hydrogen is still a bottleneck in its practical applications.Chemical hydrides(such as NaBH_(4),NH_(3)BH_(3),N_(2)H_(4)·H_(2)O,N_(2)H_(4)BH_(3),and HCOOH)are considered as potential chemical hydrogen storage materials that can achieve rapid on-site hydrogen production.At present,the most critical issue for them is to develop economic catalysts to achieve efficient hydrogen production from chemical hydrides.Cop-per(Cu)is considered as a promising catalyst that is one of the most reactive metals among the first-row transition metals and economically cheap.In this review,we outline the recent advancements of Cu-based catalysts in catalyzing hydrogen production from chemical hydrides.Moreover,the synthesis methods,characterization techniques,and hydrogen production catalytic activity of Cu-based catalysts were also introduced.Finally,a brief conclusion and outlook are given for the application of Cu-based catalysts in the dehydrogenation of chemical hydrides.We hope that this review will stimulate interest in the promising research area of Cu-based catalysts for the dehydrogenation of chem-ical hydrides.
基金financially supported by the National Natural Science Foundation of China (Nos.21868016, 21763018,22005296 and 21875096)the Key Laboratory for Environment and Energy Catalysis of Jiangxi Province (No. 20181BCD40004)+1 种基金the Natural Science Foundation of Jiangxi Province (No.20181BAB203016)the Graduate Students Innovation Special Foundation of Jiangxi Province (No.YC2021-B014)。
文摘The catalytic performance is highly related to the catalyst structure.Herein,a series of Ni nanoparticles supported on Y_(2)O_(3) with different morphologies were successfully synthesized via hydrothermal process screening different pH environments.These Ni/Y_(2)O_(3)catalysts were applied to efficiently produce CO_(x)-free H2through ammonia decomposition.We identify a significant impact of Y_(2)O_(3)supports on nickel nanoclusters sizes and dispersion.The experimental results show that Ni/Y11 catalyst achieves 100% ammonia decomposition conversion under a gas hour space velocity(GHSV) of 12,000 ml·h^(-1)·gcat^(-1) and temperature of 650℃.Such a high level of activity over Ni/Y11 catalyst was attributed to a large specific surface area,appropriate alkalinity,and small Ni nanoparticles diameter with high dispersion.
基金financially supported by the National Natural Science Foundation of China (Nos. 22162013 and 22162014)Natural Science Foundation of Jiangxi Province (No. 20212ACB204009)+2 种基金the Program of the Academic and Technical Leaders of Major Disciplines of Jiangxi Province (No. 20212BCJL23059)the Thousand Talents Plan of Jiangxi Provincethe Open Project Program of State-Province Joint Engineering Laboratory of Zeolite Membrane Materials of China (No. SPJELZMM-202210)。
文摘Developing efficient and highly selective catalyst to promote hydrogen generation from hydrous hydrazine(N_(2)H_(4)·H_(2)O) and hydrazine borane(N_(2)H_(4)BH_(3))remains a challenging issue for fuel cell-based hydrogen economy.In this work,ultrafine and well-dispersed bimetallic NiPt nanoparticles(3.4 nm) were successfully immobilized on Y_(2)O_(3)-functionalized graphene(Y_(2)O_(3)/rGO) without any surfactant by a simple liquid impregnation approach.It is firstly found that integration of graphene and Y_(2)O_(3) not only can facilitate the formation of ultrafine NiPt nanoparticles(NPs),but also can effectively modulate the electronic structure of NiPt NPs,thereby boosting the catalytic performance.Compared with NiPt/Y_(2)O_(3) and NiPt/rGO,the NiPt/Y_(2)O_(3)/rGO nanocomposites(NCs) show remarkable enhanced catalytic efficiency for hydrogen production from N_(2)H_(4)-H_(2)O.In particular,the optimized Ni_(0.6)Pt_(0.4/)Y_(2)O_(3)/rGO NCs display the best catalytic efficiency and 100% H_(2) selectivity for N_(2)H_(4)-H_(2)O dehydrogenation,providing a turnover frequency(TOF) of2182 h^(-1) at 323 K,which is among the highest values ever reported.Moreover,the Ni_(0.6)Pt_(0.4)/Y_(2)O_(3)/rGO NCs also exhibit an excellent catalytic performance(TOF=3191 h^(-1)) and 100% H_(2) selectively for N_(2)H_(4)BH_(3)dehydrogenation at 323 K.The outstanding catalytic results obtained provide more possibilities for the potential applications of N_(2)H_(4)·H_(2)O and N_(2)H_(4)BH_(3) as promising chemical hydrogen storage materials.
文摘Development of low-cost and high-performance catalysts for hydrogen generation via hydrolysis of ammonia borane （NH3BH3, AB） is a highly desirable pathway for future hydrogen utilization. In this work, Ni nanocatalysts doped with CeOx and supported on graphene （Ni-CeOdgraphene） were synthesized via a facile chemical reduction route and applied as robust catalysts for the hydrolysis of AB in aqueous solution at room temperature. The as-synthesized Ni-CeOdgraphene nanocomposites （NCs） exhibited excellent catalytic activity with a turnover frequency （TOF） as high as 68.2 min-1, which is 49-fold higher than that for a simple Ni nanoparticle catalyst and is among the highest values reported for non-noble metal catalysts in AB hydrolysis. The development of efficient and low-cost Ni-CeOdgraphene catalysts enhances the feasibility of using ammonia borane as a chemical hydrogen storage material, which may find application in a hydrogen fuel-cell based economy.
基金financially supported by the National Natural Science Foundation of China(Nos.21763012,22072183,51802157 and 52001079)Changsha Municipal Natural Science Foundation(No.kq2014119)+5 种基金the International Cooperation Program of Jiangsu Province(No.BZ2020063)the Fundamental Research Funds for the Central Universities(No.30921011216)the Natural Science Foundation of Guangxi Province(No.2019GXNSFBA185004)the Civil Aviation Administration of China(No.U1933109)the Project of Education Department of Jilin Province(No.JJKH20210827KJ)Tianjin Natural Science Foundation(No.20JCZDJC00160)。
文摘Hydrogen has been always the hot topic,which drives a lot of researchers to study and explore hydrogenrelated projects and fields.The first subfield is hydrogen production with green and cost-effective means.Some methods have been intensively used for high-efficient hydrogen production,i.e.,catalytic chemical hydrogen generation,electrocatalytic hydrogen evolution,photocatalytic hydrogen evolution,photo-electrocatalytic hydrogen evolution.Most of them are driven by various catalysts.Moreover,the hydrogen storage is also an important question,which is also a present research hot topic,although the history is long with several decades.Hydrogen fuel cells have also obtained great attention due to the zero emissions.The related research mainly focuses on the cell systems and electrocatalysts used.Under this background,we invite some excellent research groups to write this progress on hydrogen from production to utilizations.Finally,we believe that this roadmap on hydrogen can give some useful guidance in future research.
基金financially supported by the National Natural Science Foundation of China (Nos. 21763012, 22162014)Scientific Research Foundation of Graduate School of Jiangxi Province(No. YC2020-B067)。
文摘Formic acid (FA), which can be produced via CO_(2) reduction and biomass conversion, has received extensive interest as a convenient and safe hydrogen carrier due to its wide range of sources, renewable, high hydrogen content (4.4 wt%), and convenient storage/transportation. Designing highly efficient catalysts is the main challenge to realize the hydrogen production from FA. In this work, well-dispersed and electron-rich PdIr alloy nanoparticles with a size of 1.8 nm are confined in amino-modified 3D mesoporous silica KIT-6 and applied as a highly efficient catalyst for robust hydrogen production from FA at ambient temperature. Small PdIr alloy nanoparticles confined by amino-modified KIT-6 (PdIr/KIT-6-NH_(2)) lead to better catalytic activity compared to that of Pd/KIT-6-NH_(2) and PdIr confined by bare KIT-6, achieving a high turnover frequency (TOF) value of 3533 h-1 at ambient temperature (303 K), 100% H_(2) selectivity and conversion toward the dehydrogenation of FA, which is comparable to the best heterogeneous catalysts ever reported. The high catalytic activity of PdIr/KIT-6-NH_(2) can be attributed to the synergistic effect between Pd and Ir, strong interaction between PdIr and KIT-6-NH_(2), as well as the amino-groups of KIT-6-NH_(2) which can act as a proton scavenger to promote the breaking of O-H bond of formic acid.
