Light-Induced Dynamic Restructuring of Cu Active Sites on TiO2 for Low-Temperature H2 Production from Methanol and Water DOI
Shunqin Luo, Hui Song, Fumihiko Ichihara

et al.

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(37), P. 20530 - 20538

Published: Sept. 7, 2023

The structure and configuration of reaction centers, which dominantly govern the catalytic behaviors, often undergo dynamic transformations under conditions, yet little is known about how to exploit these features favor functions. Here, we demonstrate a facile light activation strategy over TiO2-supported Cu catalyst regulate restructuring active sites during low-temperature methanol steam reforming. Under illumination, thermally deactivated Cu/TiO2 undergoes structural restoration from inoperative Cu2O originally metallic caused by photoexcited charge carriers TiO2, thereby leading substantially enhanced activity stability. Given low-intensity solar irradiation, optimized displays H2 production rate 1724.1 μmol g-1 min-1, outperforming most conventional photocatalytic thermocatalytic processes. Taking advantages strong light-matter-reactant interaction, achieve in situ manipulation sites, suggesting feasibility for real-time functionalization catalysts.

Language: Английский

Maximizing the synergistic effect between Pt0 and Ptδ+ in a confined Pt-based catalyst for durable hydrogen production DOI

Zilong Shao,

Shunan Zhang, Xiaofang Liu

et al.

Applied Catalysis B Environment and Energy, Journal Year: 2022, Volume and Issue: 316, P. 121669 - 121669

Published: June 28, 2022

Language: Английский

Citations

59
The Nature of Interfacial Catalysis over Pt/NiAl2O4 for Hydrogen Production from Methanol Reforming Reaction DOI
Xiuyi Wang, Didi Li, Zirui Gao

et al.

Journal of the American Chemical Society, Journal Year: 2022, Volume and Issue: 145(2), P. 905 - 918

Published: Dec. 28, 2022

Reforming of methanol is one the most favorable chemical processes for on-board H2 production, which alleviates limitation storage and transportation. The important catalytic systems reacting with water are interfacial catalysts including metal/metal oxide metal/carbide. Nevertheless, assessment on reaction mechanism active sites these still controversial. In this work, by spectroscopic, kinetic, isotopic investigations, we established a compact cascade model (ca. Langmuir–Hinshelwood model) to describe activation over Pt/NiAl2O4. We show here that reforming experiences dehydrogenation followed water–gas shift (WGS), in two separated kinetically relevant steps have been identified, is, C–H bond rupture within methoxyl adsorbed interface O–H OlH (Ol: oxygen-filled surface vacancy), respectively. addition, reactions were primarily determined abundant intermediates, CO species NiAl2O4 Pt, More importantly, excellent performance benefits from following bidirectional spillover since vacancies support considered as real component WGS reaction, These findings provide deep insight into process well during catalysis, may guide design new systems.

Language: Английский

Citations

48
Hydrogenolysis of Lignin Model Compounds on Ni Nanoparticles Surrounding the Oxygen Vacancy of CeO2 DOI
Jin Xie, Yongjie Xi, Wensheng Gao

et al.

ACS Catalysis, Journal Year: 2023, Volume and Issue: 13(14), P. 9577 - 9587

Published: July 6, 2023

The cleavage of C–O bonds presents the crucial step for realizing depolymerization lignin. Herein, we report that Ni nanoparticles (NiNPs) supported on CeO2 with oxygen vacancies (Ov) show high activity and selectivity in hydrogenolysis diphenyl ether (DPE, a lignin model compound), while single-site (SSNi) is nearly inactive reaction. Temperature-programmed desorption (TPD) demonstrates both DPE H2 can be adsorbed activated NiNPs. Density functional theory (DFT) calculation further indicates NiNPs are more reactive because Ov at interface between greatly enhance adsorption DPE, but no SSNi was observed. It identified atoms neighboring catalytic sites Ni/CeO2 catalyst efficient compounds. This work highlights act as active rupturing models, which conducive to rational design metal-supported catalysts, especially biomass conversion.

Language: Английский

Citations

42
Adsorption of Molecules on Defective CeO2 for Advanced Catalysis DOI
Sai Zhang, Zhimin Tian, Yuanyuan Ma

et al.

ACS Catalysis, Journal Year: 2023, Volume and Issue: 13(7), P. 4629 - 4645

Published: March 22, 2023

Adsorption of molecules on active sites heterogeneous catalysts significantly affects their catalytic performance, which provides a perspective to understand the process/mechanism at atomic level and establish structure–function relationships. This Perspective illustrates strong correlation between adsorption reactants CeO2-based improved activity and/or selectivity for various transformations. Regulating oxygen defect CeO2 an effective approach construct two typical frustrated Lewis pair (FLP) dual-active site. Benefiting from unique spatial electronic structures, FLP exhibit "embedded" configuration small molecules, promoting activation transformation. The constructed by metal clusters vacancy could break competitive thereafter enable highly selective hydrogenations. Finally, possibilities challenges in behaviors are outlined. tailorability strength anticipated stimulate guide design high-performing catalysts.

Language: Английский

Citations

39
Light-Induced Dynamic Restructuring of Cu Active Sites on TiO2 for Low-Temperature H2 Production from Methanol and Water DOI
Shunqin Luo, Hui Song, Fumihiko Ichihara

et al.

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(37), P. 20530 - 20538

Published: Sept. 7, 2023

The structure and configuration of reaction centers, which dominantly govern the catalytic behaviors, often undergo dynamic transformations under conditions, yet little is known about how to exploit these features favor functions. Here, we demonstrate a facile light activation strategy over TiO2-supported Cu catalyst regulate restructuring active sites during low-temperature methanol steam reforming. Under illumination, thermally deactivated Cu/TiO2 undergoes structural restoration from inoperative Cu2O originally metallic caused by photoexcited charge carriers TiO2, thereby leading substantially enhanced activity stability. Given low-intensity solar irradiation, optimized displays H2 production rate 1724.1 μmol g-1 min-1, outperforming most conventional photocatalytic thermocatalytic processes. Taking advantages strong light-matter-reactant interaction, achieve in situ manipulation sites, suggesting feasibility for real-time functionalization catalysts.

Language: Английский

Citations

39