...
首页> 外文期刊>Proceedings of the National Academy of Sciences of the United States of America >Highly efficient and robust molecular ruthenium catalysts for water oxidation
【24h】

Highly efficient and robust molecular ruthenium catalysts for water oxidation

机译:用于水氧化的高效耐用的分子钌催化剂

获取原文
获取原文并翻译 | 示例
           

摘要

Water oxidation catalysts are essential components of light-driven water splitting systems, which could convert water to H_2 driven by solar radiation (H_2O + hv → 1/2O_2 + H_2). The oxidation of water (H_2O →1/2O_2 + 2H~+ +2e~-) provides protons and electrons for the production of dihydrogen (2H~+ + 2e~- → H_2), a clean-burning and high-capacity energy carrier. One of the obstacles now is the lack of effective and robust water oxidation catalysts. Aiming at developing robust molecular Ru-bda (H_2bda = 2,2 '-bipyridine-6,6-dicarboxylic acid) water oxidation catalysts, we carried out density functional theory studies, correlated the robustness of catalysts against hydration with the highest occupied molecular orbital levels of a set of ligands, and successfully directed the synthesis of robust Ru-bda water oxidation catalysts. A series of mononuc-lear ruthenium complexes [Ru(bda)L_2] (L = pyridazine, pyrimidine, and phthalazine) were subsequently synthesized and shown to effectively catalyze Ce~(Ⅳ)-driven [Ce~(Ⅳ) = Ce(NH_4)_2(NO_3)_6] water oxidation with high oxygen production rates up to 286 s~(-1) and high turnover numbers up to 55,400.
机译:水氧化催化剂是光驱动水分解系统的重要组成部分,它可以将水转化为太阳辐射(H_2O + hv→1 / 2O_2 + H_2)驱动的H_2。水的氧化(H_2O→1 / 2O_2 + 2H〜+ + 2e〜-)为质子和电子的产生提供了氢(2H〜+ + 2e〜-→H_2)的生成,这是一种清洁燃烧的高容量能量载体。现在的障碍之一是缺乏有效和坚固的水氧化催化剂。为了开发鲁棒的分子式Ru-bda(H_2bda = 2,2'-联吡啶-6,6-二羧酸)水氧化催化剂,我们进行了密度泛函理论研究,将催化剂对水合作用的鲁棒性与最高的分子轨道联系起来。水平的一组配体,并成功地指导了鲁棒的Ru-bda水氧化催化剂的合成。随后合成了一系列单核钌配合物[Ru(bda)L_2](L =哒嗪,嘧啶和邻苯二甲酰肼),并显示出有效催化Ce〜(Ⅳ)驱动的[C ~~(Ⅳ)= Ce(NH_4) )_2(NO_3)_6]的水氧化过程,氧产生速率高达286 s〜(-1),高周转率高达55,400。

著录项

  • 来源
  • 作者单位

    Department of Chemistry, School of Chemical Science and Engineering, Kungliga Tekniska Hoegskolan Royal Institute of Technology, 10044 Stockholm, Sweden;

    Division of Theorectical Chemistry and Biology, School of Biotechnology, Kungliga Tekniska Hoegskolan Royal Institute of Technology, 10691 Stockholm, Sweden,Department of Chemistry, Yale University, New Haven, CT 06520;

    Division of Theorectical Chemistry and Biology, School of Biotechnology, Kungliga Tekniska Hoegskolan Royal Institute of Technology, 10691 Stockholm, Sweden;

    Department of Chemistry, School of Chemical Science and Engineering, Kungliga Tekniska Hoegskolan Royal Institute of Technology, 10044 Stockholm, Sweden,State Key Lab of Fine Chemicals, Dalian University of Technology-Kungliga Tekniska Hoegskolan Joint Education and Research Center on Molecular Devices, Dalian University of Technology, 116024 Dalian, China;

  • 收录信息 美国《科学引文索引》(SCI);美国《生物学医学文摘》(MEDLINE);美国《化学文摘》(CA);
  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类
  • 关键词

    catalysis; density function theory; seven coordination; photosystem II; solar fuels;

    机译:催化;密度函数理论;七;协调;光系统II;太阳能;

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