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Hydriding Pd cocatalysts: An approach to giant enhancement on photocatalytic CO2 reduction into CH4
  • ISSN号:0253-9837
  • 期刊名称:《催化学报》
  • 时间:0
  • 分类:O643.32[理学—物理化学;理学—化学] X131[环境科学与工程—环境科学]
  • 作者机构:[1]Key Laboratory of the Ministry of Education for Advanced Catalysis Materials, College of Chemistry and Life Sciences, Institute of Physical and Chemistry, Zhejiang Normal University, Jinhua 321004, China, [2]Hefei National Laboratory for Physical Sciences at the Microscale, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials), School of Chemistry and Materials Science, Hefei Science Center (CAS), and National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei 230026, China
  • 相关基金:Acknowledgements This work was financially supported in part by the National Natural Science Foundation of China (Nos. 21471141, U1532135, and 21603191), CAS Key Research Program of Frontier Sciences (No. QYZDB- SSW-SLH018), Zhejiang Provincial Natural Science Foundation (No. LQ16B010001), Recruitment Program of Global Experts, and CAS Hundred Talent Program XAFS measurements were performed at the beamline BL14W1 in the Shanghai Synchrotron Radiation Facility (SSRF), China.
中文摘要:

进高增值 CH 4 的公司 2 的 Photocatalytic 减小是精力和环境危机的一个有希望的解决方案。与 cocatalysts 集成半导体能为 photocatalytic 公司 2 减小改进这些活动;然而,大多数金属 cocatalysts 主要生产公司和 H 2 。此处,我们为显著地提高公司 2 的 photocatalytic 减小进 CH 4 报导一条 cocatalyst hydridation 途径。进 PdH 0.43 的 Hydriding Pd cocatalysts 在表演改进起了一个双作用。是由我们的同位素的标记实验揭示了, PdH 0.43 氢化物 cocatalysts 减少了 H 2 进化,它压制了 H 2 生产并且便于 CO 中介的变换进最后的产品:CH 4 。同时, hydridation 支持了在 cocatalysts 上套住的电子,改进充电分离。这条途径在 Pd 上从 3.2% ~ 63.6% 在 CH 4 生产增加了 photocatalytic 选择 { 100 } 并且从 15.6% ~ 73.4% 在 Pd 上 { 111 } 。结果提供卓见进 photocatalytic 机制研究并且为向 photocatalytic 公司 2 变换设计材料介绍新机会。

英文摘要:

Photocatalytic reduction of CO2 into high value-added CH4 is a promising solution for energy and environmental crises. Integrating semiconductors with cocatalysts can improve the activities for photocatalytic CO2 reduction; however, most metal cocatalysts mainly produce CO and H2. Herein, we report a cocatalyst hydridation approach for significantly enhancing the photocatalytic reduction of CO2 into CH4. Hydriding Pd cocatalysts into PdH0.43 played a dual role in performance enhancement. As revealed by our isotopic labeling experiments, the PdH0.43 hydride cocatalysts reduced H2 evolution, which suppressed the H2 production and facilitated the conversion of the CO intermediate into the final product: CH4. Meanwhile, hydridation promoted the electron trapping on the cocatalysts, improving the charge separation. This approach increased the photocatalytic selectivity in CH4 production from 3.2% to 63.6% on Pd{100} and from 15.6% to 73.4% on Pd{111}. The results provide insights into photocatalytic mechanism studies and introduce new opportunities for designing materials towards photocatalytic CO2 conversion.

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期刊信息
  • 《催化学报》
  • 北大核心期刊(2011版)
  • 主管单位:中国科学院
  • 主办单位:中国化学会 中国科学院大连化学物理研究所
  • 主编:李灿 张涛
  • 地址:大连市沙河口区中山路457号
  • 邮编:116023
  • 邮箱:chxb@dicp.ac.cn
  • 电话:0411-84379240
  • 国际标准刊号:ISSN:0253-9837
  • 国内统一刊号:ISSN:21-1195/O6
  • 邮发代号:8-93
  • 获奖情况:
  • 第三届国家期刊奖提名奖,中国科协精品科技期刊示范项目
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  • 被引量:19199