Caudillo-Flores Uriel, Sayago Rocío, Ares-Dorado Alejandro, Fuentes-Moyado Sergio, Fernández-García Marcos, Kubacka Anna
Centro de Nanociencias y Nanotecnología, Universidad Nacional Autónoma de México, Ensenada 22800, Mexico.
Instituto de Catálisis y Petroleoquímica, CSIC, C/Marie Curie 2, Madrid 28049, Spain.
ACS Sustain Chem Eng. 2023 Feb 20;11(9):3896-3906. doi: 10.1021/acssuschemeng.2c07285. eCollection 2023 Mar 6.
In this contribution, a series of Pd-promoted Nb-doped titania samples were essayed in the gas-phase thermo-photo production of syngas from methanol/water mixtures. The Pd loading was tested in the 0.1 to 2.5 wt % range, leading to the presence of metallic nanoparticles under reaction. Reaction rates exceeding 52 mmol H g h and quantum efficiencies above 33% were obtained. The optimum sample having a 0.5 wt % of Pd provided an outstanding synergy between light and heat under reaction conditions, facilitating the boost of activity with respect to the single-source processes and achieving high selectivity to syngas. The spectroscopic analysis of the physico-chemical ground of the activity unveiled that the noble metal interaction with the Nb-doped anatase support triggers a cooperative effect, promoting the evolution of formic acid-type methanol-derived carbon-containing species and rendering a significant enhancement of syngas production. The proposed thermo-photo system is thus a firm candidate to contribute to the new green circular economy.
在本论文中,一系列钯促进的铌掺杂二氧化钛样品被用于由甲醇/水混合物气相热光生产合成气的实验。钯负载量在0.1至2.5 wt%范围内进行测试,导致反应过程中存在金属纳米颗粒。获得了超过52 mmol H g h的反应速率和高于33%的量子效率。具有0.5 wt%钯的最佳样品在反应条件下实现了光与热之间的出色协同作用,相对于单源过程促进了活性的提升,并实现了对合成气的高选择性。对活性的物理化学基础进行的光谱分析表明,贵金属与铌掺杂的锐钛矿载体之间的相互作用引发了协同效应,促进了甲酸型甲醇衍生含碳物种的演化,并显著提高了合成气的产量。因此,所提出的热光系统是助力新型绿色循环经济的有力候选者。