Hydrophobic driving fabrication of highly dispersed PtNi in Zr-doped 3D hollow flower-like MgAl2O4 spheres with abundant O vacancies for enhanced dry reforming of methane

作     者：Zhang, Chao Gao, Yongsheng Wang, Haipeng Jiang, Lulu Zhang, Delu Ming, Shujun Fu, Guangying Wang, Chao Lv, Zhiguo 

作者机构：Qingdao Univ Sci & Technol Coll Chem Engn State Key Lab Base Ecochem Engn Qingdao 266042 Peoples R China Huanggang Normal Univ Sch Chem & Chem Engn Hubei Key Lab Proc & Applicat Catalyt Mat Huangzhou 438000 Peoples R China Chinese Acad Sci Qingdao Inst Bioenergy & Bioproc Technol Qingdao 266101 Peoples R China Wuhan Univ Technol State Key Lab Adv Technol Mat Synth & Proc Wuhan 430070 Peoples R China 

出 版 物：《JOURNAL OF COLLOID AND INTERFACE SCIENCE》 (J. Colloid Interface Sci.)

年 卷 期：2025年第685卷

页      面：244-254页

核心收录：

学科分类：081704[工学-应用化学] 07[理学] 070304[理学-物理化学(含∶化学物理)] 08[工学] 0817[工学-化学工程与技术] 0703[理学-化学] 

基　　金：Natural Science Foundation of National [NSFC22208179] The 2023 Shandong Provincial Universities Youth Innovation Team Development Plan [2023KJ098] Shandong Provincial Natural Science Foundation [ZR2020ME060] State Key Laboratory of Advanced Technology for Materials Synthesis and Processing (Wuhan University of Technology) [2024-KF-17] Key Laboratory of Laser Technology and Optoelectronic Functional Mate-rials of Hainan Province [2024LTOM05] open foundation of State Key Laboratory of Chemical Engineering [SKL-ChE-24B04] Foundation of State Key Laboratory of Coal Combustion [FSKLCCA2412] Young Talent Project of Scientific Research Program of Hubei Provincial Department of Education [Q20232903] 

主　　题：PtNi alloy Carbon deposition resistance Oxygen vacancies Methane dry reforming 

摘      要：The dry reforming of methane (DRM) could convert CH4 and CO2 into syngas, offering potential for greenhouse gas mitigation. However, DRM catalyst sintering and carbon deposition remain major obstacles. In this study, a highly dispersed PtNi alloy@Zr-doped 3D hollow flower-like MgAl2O4 (AMO) spheres was prepared through a hydrophobic driving strategy. During a 50-hour test at 550 degrees C, the catalyst exhibited no significant decline in CH4 and CO2 conversion rates, demonstrating its excellent anti-sintering and anti-coking performance. The unique anti-coking performance can be attributed to Zr-induced oxygen vacancies, which enhance oxygen mobility and reduce carbon deposition. Besides, doped Zr increases basic active sites, enhancing CO2 adsorption and activation, thus accelerating carbon species conversion. At 700 degrees C, the unique synergy between highly dispersed Pt and Ni enabled CH4 and CO2 conversion rates to reach 67.5 % and 73.8 %, respectively. The incorporation of Pt or Zr extends the Ni-Ni bond and partially coordinates with Ni, enhancing the stability of the Ni lattice. The reaction of CH4 and CO2 follows the Langmuir-Hinshelwood (L-H) mechanism, where both reactant molecules are adsorbed and activated on the metallic sites. Moreover, the effective energy barrier for the CH oxidation pathway is lower by 0.16 eV than that for the C oxidation pathway, which helps suppress the formation of carbon deposits.