Scholarlink

<p>The hydrogenation of CO<sub>2</sub> to methanol is a promising route for carbon capture and utilization, however achieving high selectivity and productivity remains a challenge. This study presents a novel catalyst synthesized by pyrolyzing a zirconium-based metal-organic framework impregnated with indium, yielding ultrafine In<sub>2</sub>O<sub>3</sub> nanoparticles uniformly embedded within a ZrO<sub>2</sub> and carbon matrix. The resulting In<sub>2</sub>O<sub>3</sub>/ZrO<sub>2</sub> heterojunction exhibited abundant oxygen vacancies at the interface, which is crucial for enhancing the catalytic performance. Under gas-phase conditions, the catalyst achieves an exceptional methanol selectivity of 81% with a record-high productivity of 2.64 gMeOH·gcat⁻¹·h⁻¹ at mild reaction conditions, while in liquid-phase hydrogenation, methanol selectivity reaches 96%. Comprehensive structural characterizations confirmed that oxygen vacancies and the heterointerface served as active sites, facilitating CO<sub>2</sub> activation and methanol stabilization. Mechanistic insights from in-situ DRIFTS and ATR-IR spectroscopy revealed that methanol formation proceeds via the formate pathway, further supported by in-situ ambient-pressure X-ray photoelectron spectroscopy, demonstrating electronic structural modulation and an increased concentration of oxygen vacancies. These findings underscore the critical role of defect engineering in optimizing CO<sub>2</sub> hydrogenation catalysts and provide a pathway for designing highly efficient systems for sustainable methanol production.</p>

错误：搜索内容不能为空，请输入英文关键词
错误：关键词超出字数限制，请精简
高级检索

Metal organic framework derived In2O3/ZrO2 heterojunctions with interfacial oxygen vacancies for highly selective CO2-to-methanol hydrogenation

  • 期刊论文

  • 出版模式：

    开放获取

  • 发表日期：

    2025年10月7日

查看全文
  • Paramita Koley,
  • Subhash Chandra Shit,
  • Takefumi Yoshida,
  • Deshetti Jampaiah,
  • Hiroko Ariga-Miwa,
  • Tomoya Uruga,
  • Jyotishman Kaishyop,
  • Tayebeh Hosseinnejad,
  • Selvakannan Periasamy,
  • Ravindra D. Gudi,
  • Dharmendra D. Mandaliya,
  • Yasuhiro Iwasawa,
  • Suresh K. Bhargava

摘要

The hydrogenation of CO2 to methanol is a promising route for carbon capture and utilization, however achieving high selectivity and productivity remains a challenge. This study presents a novel catalyst synthesized by pyrolyzing a zirconium-based metal-organic framework impregnated with indium, yielding ultrafine In2O3 nanoparticles uniformly embedded within a ZrO2 and carbon matrix. The resulting In2O3/ZrO2 heterojunction exhibited abundant oxygen vacancies at the interface, which is crucial for enhancing the catalytic performance. Under gas-phase conditions, the catalyst achieves an exceptional methanol selectivity of 81% with a record-high productivity of 2.64 gMeOH·gcat⁻¹·h⁻¹ at mild reaction conditions, while in liquid-phase hydrogenation, methanol selectivity reaches 96%. Comprehensive structural characterizations confirmed that oxygen vacancies and the heterointerface served as active sites, facilitating CO2 activation and methanol stabilization. Mechanistic insights from in-situ DRIFTS and ATR-IR spectroscopy revealed that methanol formation proceeds via the formate pathway, further supported by in-situ ambient-pressure X-ray photoelectron spectroscopy, demonstrating electronic structural modulation and an increased concentration of oxygen vacancies. These findings underscore the critical role of defect engineering in optimizing CO2 hydrogenation catalysts and provide a pathway for designing highly efficient systems for sustainable methanol production.