...
  • 主题
高级搜索  >
历史搜索 清空历史
首页> 外文期刊>The journal of physical chemistry, C. Nanomaterials and interfaces >Visible-Light-Driven Photoproduction of Hydrogen Using Rhodium Catalysts and Platinum Nanoparticles with Formate
【24h】

Visible-Light-Driven Photoproduction of Hydrogen Using Rhodium Catalysts and Platinum Nanoparticles with Formate

机译：铑催化剂和甲酰胺铂纳米颗粒的可见光驱动氢光生产

获取原文
获取原文并翻译 | 示例
           
页面导航
  • 摘要
  • 著录项
  • 相似文献
  • 相关主题

摘要

Photochemical hydrogen production is carried out using molecular Rh complexes and sodium formate in the presence of platinum nanoparticles (PtNPs) in aqueous buffer solution. Visible-light-driven photo catalytic reactions for hydrogen production with and without nicotinamide adenine dinucleotide (NAD~+) follow two different pathways. Complex [Cp~*Rh- (bpy)(OH2)]~(2+) selectively reduces NAD~+ to generate NADH using formate as a proton and electron donor and the chemically generated NADH is sequentially used by PtNPs upon photoactivation of eosin Y to produce hydrogen. However, hydrogen is also produced in photoreactions of the Rh catalyst and PtNPs with formate in the absence of NAD~+ and eosin Y. The second pathway for hydrogen production was performed under the conditions without NAD~+ and eosin Y and derived from a direct electron transfer from in situ generated rhodium (III)-hydride species to photoexcited PtNPs. The direct electron transfer from the rhodium-hydride species to visible-light-driven PtNPs was first observed in this study. These two pathways for hydrogen production showed different rate-limiting steps based on a Hammett plot using Rh catalysts containing electron-donating and electron-withdrawing groups. Kinetic isotope effects as well as Hammett plot supported the rate-limiting step of the NADH generation for the first pathway of hydrogen production and the Rh—H formation for the second pathway.
机译：在缓冲水溶液中存在铂纳米颗粒（PtNPs）的情况下，使用分子Rh络合物和甲酸钠进行光化学制氢。在有和没有烟酰胺腺嘌呤二核苷酸（NAD〜+）的情况下，可见光驱动的光催化生产氢气的反应遵循两种不同的途径。络合物[Cp〜* Rh-（bpy）（OH2）]〜（2+）使用甲酸作为质子和电子供体，选择性还原NAD〜+以生成NADH，并且曙红Y的光活化后由PtNP顺序使用化学生成的NADH产生氢气。但是，在不存在NAD〜+和曙红Y的情况下，Rh催化剂和PtNPs与甲酸酯的光反应中也会产生氢。第二条产生氢的途径是在没有NAD〜+和曙红Y的条件下进行的，并且直接来源于电子从原位生成的氢化铑（III）物质转移至光激发的PtNP。在这项研究中首次观察到从氢化铑物质到可见光驱动的PtNPs的直接电子转移。基于使用含有给电子和吸电子基团的Rh催化剂的Hammett图，这两个产氢途径显示出不同的限速步骤。动力学同位素效应以及哈米特图支持了第一个产氢途径的NADH生成和第二个途径的Rh-H形成的限速步骤。

著录项

相似文献

  • 外文文献
  • 中文文献
  • 专利
获取原文

客服邮箱：kefu@zhangqiaokeyan.com

京公网安备：11010802029741号 ICP备案号：京ICP备15016152号-6 六维联合信息科技 (北京) 有限公司©版权所有

  • 客服微信

  • 服务号