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From Ru-bda to Ru-b...
From Ru-bda to Ru-bds : a step forward to highly efficient molecular water oxidation electrocatalysts under acidic and neutral conditions
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- Yang, Jing (författare)
- Southern Univ Sci & Technol, Shenzhen Grubbs Inst, Dept Chem, Shenzhen 518055, Peoples R China.;Southern Univ Sci & Technol, Guangdong Prov Key Lab Energy Mat Elect Power, Shenzhen 518055, Peoples R China.
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- Wang, Lei (författare)
- KTH,Organisk kemi
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- Zhan, Shaoqi (författare)
- KTH,Teoretisk kemi och biologi
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- Zou, Haiyuan (författare)
- Southern Univ Sci & Technol, Shenzhen Grubbs Inst, Dept Chem, Shenzhen 518055, Peoples R China.;Southern Univ Sci & Technol, Guangdong Prov Key Lab Energy Mat Elect Power, Shenzhen 518055, Peoples R China.
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- Chen, Hong (författare)
- Southern Univ Sci & Technol, Sch Environm Sci & Engn, Shenzhen 518055, Peoples R China.
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- Ahlquist, Mårten S. G., 1979- (författare)
- KTH,Teoretisk kemi och biologi
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- Duan, Lele (författare)
- Southern Univ Sci & Technol, Shenzhen Grubbs Inst, Dept Chem, Shenzhen 518055, Peoples R China.;Southern Univ Sci & Technol, Guangdong Prov Key Lab Energy Mat Elect Power, Shenzhen 518055, Peoples R China.;Dalian Univ Technol DUT, DUT KTH Joint Educ & Res Ctr Mol Devices, State Key Lab Fine Chem, Dalian 116012, Peoples R China.
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- Sun, Licheng, 1962- (författare)
- KTH,Organisk kemi,Dalian Univ Technol DUT, DUT KTH Joint Educ & Res Ctr Mol Devices, State Key Lab Fine Chem, Dalian 116012, Peoples R China.;Westlake Univ, Sch Sci, Ctr Artificial Photosynth Solar Fuels, Hangzhou 310024, Peoples R China.
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Southern Univ Sci & Technol, Shenzhen Grubbs Inst, Dept Chem, Shenzhen 518055, Peoples R China;Southern Univ Sci & Technol, Guangdong Prov Key Lab Energy Mat Elect Power, Shenzhen 518055, Peoples R China. Organisk kemi (creator_code:org_t)
- 2021-01-14
- 2021
- Engelska.
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Ingår i: Nature Communications. - : Springer Nature. - 2041-1723. ; 12:1
- Relaterad länk:
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https://doi.org/10.1...
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https://www.nature.c...
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https://urn.kb.se/re...
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https://doi.org/10.1...
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Abstract
Ämnesord
Stäng
- Significant advances during the past decades in the design and studies of Ru complexes with polypyridine ligands have led to the great development of molecular water oxidation catalysts and understanding on the O-O bond formation mechanisms. Here we report a Ru-based molecular water oxidation catalyst [Ru(bds)(pic)(2)] (Ru-bds; bds(2-) = 2,2-bipyridine-6,6 ' -disulfonate) containing a tetradentate, dianionic sulfonate ligand at the equatorial position and two 4-picoline ligands at the axial positions. This Ru-bds catalyst electrochemically catalyzes water oxidation with turnover frequencies (TOF) of 160 and 12,900s(-1) under acidic and neutral conditions respectively, showing much better performance than the state-of-art Ru-bda catalyst. Density functional theory calculations reveal that (i) under acidic conditions, the high valent Ru intermediate Ru-V=O featuring the 7-coordination configuration is involved in the O-O bond formation step; (ii) under neutral conditions, the seven-coordinate Ru-IV=O triggers the O-O bond formation; (iii) in both cases, the I2M (interaction of two M-O units) pathway is dominant over the WNA (water nucleophilic attack) pathway. Developing efficient molecular water oxidation catalysts for artificial photosynthesis is a challenging task. Here the authors introduce a ruthenium based complex with negatively charged sulfonate groups to effectively drive water oxidation under both acidic and neutral conditions.
Ämnesord
- NATURVETENSKAP -- Kemi -- Organisk kemi (hsv//swe)
- NATURAL SCIENCES -- Chemical Sciences -- Organic Chemistry (hsv//eng)
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