Amine-functionalized hierarchically porous carbon supported Pd nanocatalysts for highly efficient H2 generation from formic acid with fast-diffusion channels  

作　　者：Xianzhao Shao Xinyi Miao Fengwu Tian Miaomiao Bai Xiaosha Guo Wei Wang Zuoping Zhao Xiaohui Ji Miyi Li Fangan Deng 

机构地区：[1]Shaanxi Key Laboratory of Catalysis,School of Chemistry and Environment Science,Shanxi University of Technology,Hanzhong 723001,Shaanxi,China [2]School of Mathematics and Computer Science,Shanxi University of Technology,Hanzhong 723001,Shaanxi,China [3]State Key Laboratory of Qinba Bio-Resource and Ecological Environment,Shaanxi University of Technology,Hanzhong 723001,Shaanxi,China [4]School of Chemistry and Chemical Engineering,Beijing Institute of Technology,Beijing 102488,China

出　　处：《Journal of Energy Chemistry》2023年第1期249-258,I0007,共11页能源化学（英文版）

基　　金：funded by the Natural Science Basic Research Program of Shaanxi(2021JCW-20);the Key Research and Development Program of Shaanxi(2020ZDLGY11-06);the Scientific Research Plan Projects of Shaanxi Education Department(20JS014);the Scientific Research Project of City-University Co-construction of Shaanxi Province(SXC-2108)。

摘　　要：Formic acid(FA)has come to be considered a potential candidate for hydrogen storage,and the development of efficient catalysts for H2releasing is crucial for realizing the sustainable process from FA.Herein,we have developed the ultrafine Pd nanoparticle(NPs)with amine-functionalized carbon as a support,which was found to show an excellent catalytic activity in H_(2)generation from FA dehydrogenation.The synergetic mechanism between amine-group and Pd active site was demonstrated to facilitate H2generation byβ-hydride elimination.Moreover,the texture of support for Pd NPs also plays an important role in determining the reactivity of FA,since the diffusion of gaseous products makes the kinetics of diffusion as a challenge in this high performance Pd catalysts.As a result,the as-prepared Pd/NH_(2)-TPC catalyst with the small sized Pd nanoparticles and the hierarchically porous structures shows a turnover of frequency(TOF)value of 4312 h^(-1)for the additive-free FA dehydrogenation at room temperature,which is comparable to the most promising heterogeneous catalysts.Our results demonstrated that the intrinsic catalytic activities of active site as well as the porous structure of support are both important factors in determining catalytic performances in H2generation from FA dehydrogenation,which is also helpful to develop high-activity catalysts for other advanced gas-liquid-solid reactions systems.

关 键 词：Hierarchically carbon Diffusion Formic acid Hydrogen production Palladium nanoparticles 

分 类 号：O643.36[理学—物理化学]