Modulating Pt States through Hydroxyl Control for Low-Temperature Aqueous Phase Reforming of Methanol

被引:1
作者
Yang, Yuyao [1 ,2 ]
Bie, Xuan [1 ,2 ]
Qi, Xiaoying [1 ,2 ]
Xu, Yongqing [1 ,2 ]
Li, Qinghai [1 ,2 ]
Zhang, Yanguo [1 ,2 ]
Zhou, Hui [1 ,2 ]
机构
[1] Tsinghua Univ, Dept Energy & Power Engn, Key Lab Thermal Sci & Power Engn, Beijing Key Lab CO2 Utilizat & Reduct Technol,Mini, Beijing 100084, Peoples R China
[2] Tsinghua Univ, Shanxi Res Inst Clean Energy, Taiyuan 030000, Shanxi, Peoples R China
基金
北京市自然科学基金; 中国国家自然科学基金;
关键词
hydroxyl; aqueous phase reforming of methanol; Al2O3; hydrogen; five-coordinatedAl; hydrogen bond donor; HYDROGEN; CATALYSTS; VACANCIES; PLATINUM; SURFACE; WATER;
D O I
10.1021/acscatal.5c00357
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Aqueous phase reforming of methanol (APRM) offers a method for releasing H-2 from the liquid phase, by which H-2 can be stored in methanol safely. It is an efficient way to design high-performance catalysts by controlling the hydroxyl (OH) groups, but its mechanism for affecting the APRM is still unclear. Herein, we loaded Pt on three types of Al2O3 (nanopolyhedron, nanosheet, and nanorod Al2O3) with different OH contents and types. Among them, Pt/nanorod Al2O3 exhibited the highest H-2 production rate of 20.4 mu mol g(-1) s(-1) with 96.6% H-2 selectivity at a low temperature of 190 degrees C. This was attributed to the roles of hydroxyl groups in modulating Pt states. On nanopolyhedron, nanosheet, and nanorod Al2O3, the bonding of Pt with O atoms became more favorable as the dehydroxylation happened. In particular, on nanorod Al2O3, the dehydroxylation process generated a high density of five-coordinated Al (AlV) sites, facilitating the dispersion and anchoring of Pt particles. Moreover, the special OH groups (hydrogen bond donor) on nanorod Al2O3 promoted Pt particle reduction via the movement of electrons. Ultimately, the results demonstrated the influence of OH groups on the dispersion and reduction of active metals, offering perspectives for designing catalysts for APRM through hydroxyl control.
引用
收藏
页码:5847 / 5857
页数:11
相关论文
共 47 条
[1]   HYDROGEN-OXYGEN TITRATION METHOD FOR MEASUREMENT OF SUPPORTED PLATINUM SURFACE AREAS [J].
BENSON, JE ;
BOUDART, M .
JOURNAL OF CATALYSIS, 1965, 4 (06) :704-&
[2]   Fabrication of Ce-ReS2 by Molten Salt for Electrochemical Hydrogen Evolution [J].
Chen, Ran ;
Ma, Minghai ;
Luo, Yi ;
Qian, Liping ;
Wan, Shunli ;
Xu, Shengyou ;
She, Xinsong .
TRANSACTIONS OF TIANJIN UNIVERSITY, 2022, 28 (06) :440-445
[3]   Evolution of Structure and of Grafting Properties of γ-Alumina with Pretreatment Temperature [J].
Delgado, Marco ;
Delbecq, Francoise ;
Santini, Catherine C. ;
Lefebvre, Frederic ;
Norsic, Sebastien ;
Putaj, Piotr ;
Sautet, Philippe ;
Basset, Jean-Marie .
JOURNAL OF PHYSICAL CHEMISTRY C, 2012, 116 (01) :834-843
[4]   Hierarchical Hexagonal Zeolites: Intrinsic Transformation Directed by Precise Control of Synthetic Conditions [J].
Ding, He ;
Xiao, Zixing ;
Zhang, Jingshuang ;
Fu, Tianyi ;
Bai, Peng ;
Guo, Xianghai .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2018, 57 (15) :5282-5290
[5]   Surface Hydroxyl-Determined Migration and Anchoring of Silver on Alumina in Oxidative Redispersion [J].
Fan, Yamei ;
Wang, Fei ;
Li, Rongtan ;
Liu, Conghui ;
Fu, Qiang .
ACS CATALYSIS, 2023, 13 (04) :2277-2285
[6]   Aqueous Phase Methanol Reforming Catalyzed by Fe-Cu Alloy Nanoparticles Wrapped on Nitrogen-Doped Graphene [J].
Garcia-Baldovi, Alberto ;
Peng, Lu ;
Santiago-Portillo, Andrea ;
Asiri, Abdullah M. ;
Primo, Ana ;
Garcia, Hermenegildo .
ACS APPLIED ENERGY MATERIALS, 2022, 5 (07) :9173-9180
[7]   Dual active sites engineering of electrocatalysts for alkaline hydrogen evolution [J].
Gou, Wankun ;
Sun, Hongming ;
Cheng, Fangyi .
NANO RESEARCH ENERGY, 2024, 3 (03)
[8]   New approaches to hydrogen storage [J].
Graetz, Jason .
CHEMICAL SOCIETY REVIEWS, 2009, 38 (01) :73-82
[9]   Methanol steam reforming for hydrogen production driven by an atomically precise Cu catalyst [J].
Hu, Weigang ;
Liu, Haoqi ;
Zhang, Yuankun ;
Ji, Jiawei ;
Li, Guangjun ;
Cai, Xiao ;
Liu, Xu ;
Xu, Wen Wu ;
Ding, Weiping ;
Zhu, Yan .
GREEN ENERGY & ENVIRONMENT, 2024, 9 (07) :1079-1084
[10]   Site-Dependent Lewis Acidity of γ-Al2O3 and Its Impact on Ethanol Dehydration and Etherification [J].
Jenness, Glen R. ;
Christiansen, Matthew A. ;
Caratzoulas, Stavros ;
Vlachos, Dionisios G. ;
Gorte, Raymond J. .
JOURNAL OF PHYSICAL CHEMISTRY C, 2014, 118 (24) :12899-12907