文献类型：期刊文献

英文题名：Balancing water dissociation and toluene activation via A-site La doping in LaxNiO3/CeO2 catalyst for efficient hydrogen production

作者：Peng, Ruixiao An, Tingwei Wang, Keliang Li, Ziwei Liu, Fei Li, Min

第一作者：Peng, Ruixiao

通信作者：Li, ZW[1];Liu, F[1];Li, M[1]

机构：[1]Guizhou Univ, Sch Chem & Chem Engn, Guizhou Prov Key Lab Green Chem & Clean Energy Tec, Guiyang 550025, Peoples R China;[2]PetroChina, Petrochem Res Inst, Lanzhou Petrochem Res Ctr, Lanzhou 730060, Peoples R China;[3]Guizhou Inst Technol, Sch Civil Engn, Guiyang 550003, Peoples R China;[4]Maotai Inst, Sch Brewing Engn, Renhuai 564507, Peoples R China

第一机构：Guizhou Univ, Sch Chem & Chem Engn, Guizhou Prov Key Lab Green Chem & Clean Energy Tec, Guiyang 550025, Peoples R China

通信机构：corresponding author), Guizhou Univ, Sch Chem & Chem Engn, Guizhou Prov Key Lab Green Chem & Clean Energy Tec, Guiyang 550025, Peoples R China.

年份：2026

卷号：726

外文期刊名：APPLIED CATALYSIS A-GENERAL

收录：;EI(收录号：20263421350596);Scopus(收录号：2-s2.0-105047883960);WOS:【SCI-EXPANDED(收录号:WOS:001856815600001)】；

基金：This work was supported by National Natural Science Foundation of China (22279024, 22168013), Natural Science Foundation of Guizhou (QiankehejichuMS[2025]185), Young Top Talents Program of Science and Technology of Guizhou Province (Qianjiaoji[2024]315).

语种：英文

外文关键词：Water dissociation; Toluene activation; La content tuning; Hydrogen production; Reaction mechanism

摘要：Steam reforming of toluene (SRT) represents a pivotal route for the valorization of biomass tar, with its efficacy hinging on the development of highly efficient and stable catalyst. To achieve this goal, LaxNiO3/CeO2 (X = 0.97, 1.00, 1.03) catalysts were designed via the facile sol-gel method. LaNiO3/CeO2 catalyst with moderate La content exhibits the best catalytic performance with the toluene conversion remained above 90% during the initial 15 h and over 80% with the H2 yield higher than 1700 mmol/gcat/h during the 50 h of continuous operation at 700 degrees C. This outstanding performance can be attributed to its adequate concentration of lattice oxygen, oxygen vacancy (Ov), Ni0 as well as electron density around Ni0 confirmed from the X-ray diffraction, Raman, X-ray photoelectron spectroscopy, H2O temperature-programmed surface reaction and density functional theory (DFT) calculation. These structural advantages of LaNiO3/CeO2 not only promotes water dissociation to generate active oxygen species for carbon removal but also boosts toluene activation via C-H bond cleavage. The SRT reaction mechanism over LaNiO3/CeO2 was unveiled based on the In-situ infrared spectroscopy and isotope labeling experiments as well as DFT calculations: Ni sites facilitate toluene activation (with the oxidation of C6H5-CH2* identified as the rate-determining step), while the Ov lowers the energy barrier for water dissociation. Both lattice oxygen and oxygen species derived from water participate in the reaction. This work provides new insights in obtaining good SRT catalytic performance through balancing water dissociation and toluene activation via La content tuning.