Enhanced dry reforming of methane over nickel catalysts supported on zirconia coated mesoporous silica

IF 4.6 2区综合性期刊 Q1 MULTIDISCIPLINARY SCIENCES

iScience Pub Date : 2025-05-03 DOI:10.1016/j.isci.2025.112582

Yi Zhong , Yuhao Peng , Hao Gu , Shan Zhang , Feng Ryan Wang , Wei Xiao , Hulei Yu , Dong Gu

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引用次数: 0

Abstract

Dry reforming of methane (DRM) offers a sustainable route to convert CH₄ and CO₂ into syngas, addressing both greenhouse gas emissions and energy demand. However, catalyst deactivation due to sintering and coking limits practical applications. In this work, we developed a mesoporous Ni-based catalyst (Ni/ZrSBA-15-OH) featuring abundant Ni-ZrO₂ interfaces and small Ni nanoparticles (5.6 nm) confined within a stable silica framework. This catalyst showed excellent performance, achieving 80% CH₄ and 87% CO₂ conversions at 750°C, with minimal coke formation (0.4 mg g_cat⁻¹ h⁻¹) and high durability (1.3% CH₄ conversion loss over 20 h). Advanced characterizations (X-ray absorption spectroscopy [XAS], transmission electron microscopy [TEM], H₂-temperature programmed reduction [H₂-TPR], and temperature-programmed surface reaction [TPSR]) revealed that the metal-oxide interface enhances the activation of reactants and stabilizes active sites. Density functional theory (DFT) calculations confirmed that the Ni-ZrO₂ interface increases the energy barrier for CH∗ dehydrogenation, effectively suppressing carbon deposition. This study provides a rational strategy for designing structurally robust and coke-resistant Ni-based catalysts for efficient DRM.

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氧化锆包覆介孔二氧化硅负载镍催化剂上甲烷干重整的增强

甲烷干重整（DRM）为甲烷和二氧化碳转化为合成气提供了一条可持续的途径，既解决了温室气体排放问题，又满足了能源需求。然而，由于烧结和焦化导致的催化剂失活限制了实际应用。在这项工作中，我们开发了一种介孔镍基催化剂（Ni/ zrba -15- oh），具有丰富的Ni- zro2界面和小的Ni纳米颗粒（5.6 nm），被限制在稳定的二氧化硅框架内。该催化剂表现出优异的性能，在750℃下CH4转化率为80%，CO2转化率为87%，焦炭生成量最小（0.4 mg gcat−1 h−1），耐久性高（20 h内CH4转化率损失1.3%）。高级表征（x射线吸收光谱[XAS]，透射电子显微镜[TEM]， h2 -温度程序还原[H2-TPR]和温度程序表面反应[TPSR]）表明，金属-氧化物界面增强了反应物的活性并稳定了活性位点。密度泛函理论（DFT）计算证实，Ni-ZrO2界面增加了CH∗脱氢的能垒，有效地抑制了碳沉积。本研究为设计结构坚固、耐焦炭的高效DRM镍基催化剂提供了合理的策略。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

iScience Multidisciplinary-Multidisciplinary

CiteScore

7.20

自引率

1.70%

发文量

1972

审稿时长

6 weeks

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