文献类型：期刊文献

英文题名：Exploring the key role of electronic effects in Pd catalysts supported on Ni-modified N-doped porous carbon for direct synthesis of H2O2 under atmospheric pressure

作者：Jiang, Donghai Shi, Yongyong Zhou, Liming Ma, Jun Yin, Chaochuang Lin, Qian Pan, Hongyan

第一作者：Jiang, Donghai;蒋东海

通信作者：Lin, Q[1];Pan, HY[1]

机构：[1]Guizhou Univ, Sch Chem & Chem Engn, Guiyang 550025, Guizhou, Peoples R China;[2]Guizhou Inst Technol, Sch Chem Engn, Guiyang 550003, Guizhou, Peoples R China;[3]Guizhou Univ, State Key Lab Publ Big Data, Guiyang 550025, Guizhou, Peoples R China;[4]Guizhou Key Lab Green Chem & Clean Energy Technol, Guiyang 550025, Guizhou, Peoples R China;[5]Liupanshui Normal Univ, Sch Chem & Mat Engn, Liupanshui 553004, Guizhou, Peoples R China

第一机构：Guizhou Univ, Sch Chem & Chem Engn, Guiyang 550025, Guizhou, Peoples R China

通信机构：corresponding author), Guizhou Univ, Sch Chem & Chem Engn, Guiyang 550025, Guizhou, Peoples R China.

年份：2024

卷号：565

外文期刊名：MOLECULAR CATALYSIS

收录：;EI(收录号：20243016755144);Scopus(收录号：2-s2.0-85199278470);WOS:【SCI-EXPANDED(收录号:WOS:001279850500001)】；

基金：Thanks for the computing support of the State Key Laboratory of Public Big Data, Guizhou University. This work was financially supported by National Natural Science Foundation of China (Grant No.22068009), National Natural Science Foundation of China (Grant No.22262006), Guizhou Provincial Science and Technology Projects (Grant No. QKHJC-ZK [2022]YB088), and Guizhou Provincial Basic Research Program(Natural Science) ([2022]534).

语种：英文

外文关键词：Ni modification; Pd -based catalyst; Supported catalyst; Direct synthesis of H 2 O 2; Electronic structure

摘要：Developing high-performance catalysts for direct synthesis of hydrogen peroxide (H2O2; DSHP) remains challenging. The paper proposes a strategy to optimize Pd catalysts by enriching Ni-modified N-doped porous carbon. The theoretical studies indicate that Ni modulates the electronic structure of Pd through charge transfer and strain effects, effectively reducing the adsorption energy of reaction intermediates. Furthermore, the Crystal Orbital Hamilton Population (COHP) analysis demonstrated that the energy-integrated COHP (ICOHP) of the O-O bonds in O2* (* denotes the adsorbed state), OOH*, and HOOH* were positively correlated with dissociation activation energies and negatively correlated with hydrogenation activation energies. The modulation of the electronic structure of Pd by Ni reduces the hydrogenation activation energies of O2* and OOH* and increases the dissociation activation energies of O2*, OOH*, and HOOH*, thereby enhancing the selectivity and productivity of H2O2. The experimental results aligned with the theoretical predictions, showcasing that the optimized Pd-Ni7.5/NPCs catalyst exhibited remarkable H2O2 selectivity and productivity of 70.5 % and 230.31 mol kgcat -1 & sdot;h-1, respectively, surpassing the performance of Pd/NPCs (47.1 % and 52.3 mol kgcat offers profound insights into the crucial role of electron effects in DSHP using nickel-modified palladium catalysts, providing strong evidence into the design and optimization of Pd catalysts.