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Sökning: onr:"swepub:oai:DiVA.org:kth-302712" > Isolation and Ident...

Isolation and Identification of Pseudo Seven-Coordinate Ru(III) Intermediate Completing the Catalytic Cycle of Ru-bda Type of Water Oxidation Catalysts

Liu, Tianqi (författare)
KTH,Organisk kemi,Molekylär elektronik, CMD,Department of Chemistry, School of Engineering Sciences in Chemistry, Biotechnology, and Health, KTH Royal Institute of Technology, Stockholm 10044
Li, Ge (författare)
KTH,Tillämpad fysikalisk kemi,Department of Theoretical Chemistry and Biology, School of Engineering Sciences in Chemistry, Biotechnology, and Health, KTH Royal Institute of Technology, Stockholm 10691
Shen, Nannan (författare)
State Key Laboratory of Radiation Medicine and Protection, School for Radiological and Interdisciplinary Sciences (RAD-X), Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education Institutions, Soochow University, Suzhou 215123
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Wang, Linqin (författare)
Center of Artificial Photosynthesis for Solar Fuels, School of Science, Westlake University, Hangzhou 310024
Timmer, Brian (författare)
KTH,Organisk kemi,Department of Chemistry, School of Engineering Sciences in Chemistry, Biotechnology, and Health, KTH Royal Institute of Technology, Stockholm 10044
Zhou, Shengyang (författare)
Uppsala universitet,Nanoteknologi och funktionella material
Zhang, Biaobiao (författare)
Center of Artificial Photosynthesis for Solar Fuels, School of Science, Westlake University, Hangzhou 310024
Kravchenko, Alexander (författare)
KTH,Kemi,Department of Chemistry, School of Engineering Sciences in Chemistry, Biotechnology, and Health, KTH Royal Institute of Technology, Stockholm 10044
Xu, Bo (författare)
KTH,Elektroteknisk teori och konstruktion,Department of Chemistry, School of Engineering Sciences in Chemistry, Biotechnology, and Health, KTH Royal Institute of Technology, Stockholm 10044
Ahlquist, Mårten S. G., 1979- (författare)
KTH,Teoretisk kemi och biologi,Department of Theoretical Chemistry and Biology, School of Engineering Sciences in Chemistry, Biotechnology, and Health, KTH Royal Institute of Technology, Stockholm 10691
Sun, Licheng, 1962- (författare)
KTH,Molekylär elektronik, CMD,Organisk kemi,Department of Chemistry, School of Engineering Sciences in Chemistry, Biotechnology, and Health, KTH Royal Institute of Technology, Stockholm 10044;Center of Artificial Photosynthesis for Solar Fuels, School of Science, Westlake University, Hangzhou 310024;Institute of Artificial Photosynthesis (IAP), State Key Laboratory of Fine Chemicals, Dalian University of Technology (DUT), Dalian 116024
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 (creator_code:org_t)
Chinese Chemical Society, 2022
2022
Engelska.
Ingår i: CCS Chemistry. - : Chinese Chemical Society. - 2096-5745. ; 4:7, s. 2481-2490
  • Tidskriftsartikel (refereegranskat)
Abstract Ämnesord
Stäng  
  • Isolation of RuIII-bda (17-electron specie) complex with an aqua ligand (2-electron donor) is challenging due to violation of the 18-electron rule. Although considerable efforts have been dedicated to mechanistic studies of water oxidation by the Ru-bda family, the structure and initial formation of the RuIII-bda aqua complex are still controversial. Herein, we challenge this often overlooked step by designing a pocket-shape Ru-based complex 1. The computational studies showed that 1 possesses the crucial hydrophobicity at the RuV(O) state as well as similar probability of access of terminal O to solvent water molecules when compared with classic Ru-bda catalysts. Through characterization of single-crystal structures at the RuII and RuIII states, a pseudo seven-coordinate “ready-to-go” aqua ligand with RuIII...O distance of 3.62 Å was observed. This aqua ligand was also found to be part of a formed hydrogen-bonding network, providing a good indication of how the RuIII-OH2 complex is formed.

Ämnesord

NATURVETENSKAP  -- Kemi -- Organisk kemi (hsv//swe)
NATURAL SCIENCES  -- Chemical Sciences -- Organic Chemistry (hsv//eng)
TEKNIK OCH TEKNOLOGIER  -- Nanoteknik (hsv//swe)
ENGINEERING AND TECHNOLOGY  -- Nano-technology (hsv//eng)

Nyckelord

pseudo seven-coordinate
Ru-bda
RuIII-OH2 intermediate
water oxidation
water preorganization
Engineering Science with specialization in Nanotechnology and Functional Materials

Publikations- och innehållstyp

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