Supports are commonly implemented in the industrial application of heterogeneous catalysts to improve the stability and recyclability of catalysts.The supported catalysts often show the enhanced activity and selectivi...Supports are commonly implemented in the industrial application of heterogeneous catalysts to improve the stability and recyclability of catalysts.The supported catalysts often show the enhanced activity and selectivity in various catalytic reactions.However,the specific contributions of electronic and steric effects to a catalytic system often remain elusive due to the lack of well-defined model systems.In this work,two types of uniform Pd nanocrystals covered by{111}facets in tetrahedral and octahedral shapes,respectively,are synthesized with identical chemical environment and loaded on Ti O_2supports to form hybrid structures(Pd{111}-Ti O_2)towards the application of formic acid decomposition.Our observation suggests that the polarization effect at the interface of Pd-Ti O_2enhances its activity in formic acid decomposition.Moreover,the Pd tetrahedrons-Ti O_2hybrid structure whose Pd{111}-Ti O_2interface possesses a larger angle shows higher catalytic activity,owing to the reduced steric effect as compared to Pd octahedrons-Ti O_2.This study reveals the nature of interface effects in formic acid decomposition,and provides a guidance for the related catalyst design.展开更多
Agglomerated Pd catalysts with the nano-porous structure were simply prepared by one-step reduction reaction without using any stabilizer. The Pd catalysts show a high catalytic activity for the decomposition of formi...Agglomerated Pd catalysts with the nano-porous structure were simply prepared by one-step reduction reaction without using any stabilizer. The Pd catalysts show a high catalytic activity for the decomposition of formic acid at room temperature. Among all the Pd catalysts tested, the Pdug catalyst exhibits the highest catalytic activity. Moreover, the breakthrough of the advanced catalysts is that the above agglomerated Pd catalysts can be easily separated from the liquid system to control the catalytic reaction at any time, which may further promote the practical application of formic acid as a H2 storage material.展开更多
Hydrogen production from formic acid decomposition(FAD)is a promising means of hydrogen energy storage and utilization in fuel cells.Development of efficient catalysts for dehydrogenation of formic acid is a challengi...Hydrogen production from formic acid decomposition(FAD)is a promising means of hydrogen energy storage and utilization in fuel cells.Development of efficient catalysts for dehydrogenation of formic acid is a challenging topic.The surface chemical and electronic structure of the active catalysis components is important in formic acid decomposition at room-temperature.Here,the pyrdinic-nitrogen doped catalysts from hyperbranched polyamide were prepared via in situ polymerization reaction process by using activated carbon as a support.Because of the introduction of the polymer,the particles of the catalysts were stabilized,and the average particle diameter was only 1.64 nm.Under mild conditions,the catalysts activities were evaluated for FAD.The optimized Pd-N30/C catalyst exhibited high performance achieving almost full conversion,with a turnover frequency of 3481 h^-1 at 30℃.展开更多
Hydrogen is recognized as a promising energy scours in the close future.Online hydrogen preparation from formic acid under mild reaction conditions causes extensive interests.Mo_(2)C and metal(Fe,Ni,Co,K)doped Mo_(2)C...Hydrogen is recognized as a promising energy scours in the close future.Online hydrogen preparation from formic acid under mild reaction conditions causes extensive interests.Mo_(2)C and metal(Fe,Ni,Co,K)doped Mo_(2)C on granular activated carbon(GAC)were prepared and used as heterogeneous catalysts for H2 generation from formic acid on a fixed bed reactor at 100–250°C.The formic acid conversions on doped Mo_(2)C-Me/GAC are clearly improved,especially at lower reaction temperatures.Co doping presents outstanding effect on H2 selectivity and conversion rate compared to Ni and Fe.A 56.3%formic acid conversion was reached on Mo_(2)C-Co/GAC at 100°C,which triples that on Mo_(2)C/GAC at the same temperature.At 150°C,a high formic acid conversion over 90%was reached on Mo_(2)C-Co/GAC.These long lifetime catalysts with no precious metal provide a low cost route to hydrogen production from formic acid.展开更多
基金supported in part by National Key R&D Program of China (2017YFA0207301)the National Natural Science Foundation of China (21725102, 21471141, U1532135, 21601173)+3 种基金CAS Key Research Program of Frontier Sciences (QYZDB-SSW-SLH018)CAS Interdisciplinary Innovation Team, Innovative Program of Development Foundation of Hefei Center for Physical Science and Technology (2016FXCX003)Anhui Provincial Natural Science Foundation (1608085QB24)Chinese Universities Scientific Fund(WK2310000067)
文摘Supports are commonly implemented in the industrial application of heterogeneous catalysts to improve the stability and recyclability of catalysts.The supported catalysts often show the enhanced activity and selectivity in various catalytic reactions.However,the specific contributions of electronic and steric effects to a catalytic system often remain elusive due to the lack of well-defined model systems.In this work,two types of uniform Pd nanocrystals covered by{111}facets in tetrahedral and octahedral shapes,respectively,are synthesized with identical chemical environment and loaded on Ti O_2supports to form hybrid structures(Pd{111}-Ti O_2)towards the application of formic acid decomposition.Our observation suggests that the polarization effect at the interface of Pd-Ti O_2enhances its activity in formic acid decomposition.Moreover,the Pd tetrahedrons-Ti O_2hybrid structure whose Pd{111}-Ti O_2interface possesses a larger angle shows higher catalytic activity,owing to the reduced steric effect as compared to Pd octahedrons-Ti O_2.This study reveals the nature of interface effects in formic acid decomposition,and provides a guidance for the related catalyst design.
文摘Agglomerated Pd catalysts with the nano-porous structure were simply prepared by one-step reduction reaction without using any stabilizer. The Pd catalysts show a high catalytic activity for the decomposition of formic acid at room temperature. Among all the Pd catalysts tested, the Pdug catalyst exhibits the highest catalytic activity. Moreover, the breakthrough of the advanced catalysts is that the above agglomerated Pd catalysts can be easily separated from the liquid system to control the catalytic reaction at any time, which may further promote the practical application of formic acid as a H2 storage material.
基金supported by the National Natural Science Foundation of China (21633008, 21733004, and 21603216)Jilin Province Science and Technology Development Program (20180101030JC)+2 种基金the Hundred Talents Program of Chinese Academy of Sciencesthe Recruitment Program of Foreign Experts (WQ20122200077)RFBR (18-53-53025)
文摘Hydrogen production from formic acid decomposition(FAD)is a promising means of hydrogen energy storage and utilization in fuel cells.Development of efficient catalysts for dehydrogenation of formic acid is a challenging topic.The surface chemical and electronic structure of the active catalysis components is important in formic acid decomposition at room-temperature.Here,the pyrdinic-nitrogen doped catalysts from hyperbranched polyamide were prepared via in situ polymerization reaction process by using activated carbon as a support.Because of the introduction of the polymer,the particles of the catalysts were stabilized,and the average particle diameter was only 1.64 nm.Under mild conditions,the catalysts activities were evaluated for FAD.The optimized Pd-N30/C catalyst exhibited high performance achieving almost full conversion,with a turnover frequency of 3481 h^-1 at 30℃.
基金financial support of grant from the Natural Science Funds for Young Scholar of China(Grant No.21107049)the priority academic program development of Jiangsu Higher Education Institution(PAPD).
文摘Hydrogen is recognized as a promising energy scours in the close future.Online hydrogen preparation from formic acid under mild reaction conditions causes extensive interests.Mo_(2)C and metal(Fe,Ni,Co,K)doped Mo_(2)C on granular activated carbon(GAC)were prepared and used as heterogeneous catalysts for H2 generation from formic acid on a fixed bed reactor at 100–250°C.The formic acid conversions on doped Mo_(2)C-Me/GAC are clearly improved,especially at lower reaction temperatures.Co doping presents outstanding effect on H2 selectivity and conversion rate compared to Ni and Fe.A 56.3%formic acid conversion was reached on Mo_(2)C-Co/GAC at 100°C,which triples that on Mo_(2)C/GAC at the same temperature.At 150°C,a high formic acid conversion over 90%was reached on Mo_(2)C-Co/GAC.These long lifetime catalysts with no precious metal provide a low cost route to hydrogen production from formic acid.