Bifunctional and regenerable molecular electrode for water electrolysis at neutral pH

doi:10.1039/d3ta00071k

	Bifunctional and regenerable molecular electrode for water electrolysis at neutral pH
	Das, Biswanath 1; Toledo-Carrillo, Esteban A.2; Li, Guoqi3 ; Stahle, Jonas 1; Thersleff, Thomas 4; Chen, Jianhong 4; Li, Lin3 ; Ye, Fei 2; Slabon, Adam 5; Gothelid, Mats 6; Weng, Tsu-Chien3 ; Yuwono, Jodie A.7; Kumar, Priyank V.7; Verho, Oscar 8; Karkas, Markus D.9; Dutta, Joydeep 2; Akermark, Bjorn 1
	2023
发表期刊	JOURNAL OF MATERIALS CHEMISTRY A
ISSN	2050-7488
EISSN	2050-7496
卷号	11 期号:25 页码:13331-13340
发表状态	已发表
DOI	10.1039/d3ta00071k
摘要	The instability of molecular electrodes under oxidative/reductive conditions and insufficient understanding of the metal oxide-based systems have slowed down the progress of H2-based fuels. Efficient regeneration of the electrode's performance after prolonged use is another bottleneck of this research. This work represents the first example of a bifunctional and electrochemically regenerable molecular electrode which can be used for the unperturbed production of H2 from water. Pyridyl linkers with flexible arms (-CH2-CH2-) on modified fluorine-doped carbon cloth (FCC) were used to anchor a highly active ruthenium electrocatalyst [RuII(mcbp)(H2O)2] (1) [mcbp2− = 2,6-bis(1-methyl-4-(carboxylate)benzimidazol-2-yl)pyridine]. The pyridine unit of the linker replaces one of the water molecules of 1, which resulted in RuPFCC (ruthenium electrocatalyst anchored on -CH2-CH2-pyridine modified FCC), a high-performing electrode for oxygen evolution reaction [OER, overpotential of ∼215 mV] as well as hydrogen evolution reaction (HER, overpotential of ∼330 mV) at pH 7. A current density of ∼8 mA cm−2 at 2.06 V (vs. RHE) and ∼−6 mA cm−2 at −0.84 V (vs. RHE) with only 0.04 wt% loading of ruthenium was obtained. OER turnover of >7.4 × 103 at 1.81 V in 48 h and HER turnover of >3.6 × 103 at −0.79 V in 3 h were calculated. The activity of the OER anode after 48 h use could be electrochemically regenerated to ∼98% of its original activity while it serves as a HE cathode (evolving hydrogen) for 8 h. This electrode design can also be used for developing ultra-stable molecular electrodes with exciting electrochemical regeneration features, for other proton-dependent electrochemical processes. © 2023 The Royal Society of Chemistry
关键词	Carboxylation Electrocatalysts Electrochemical electrodes Hydrogen Molecules Ruthenium Bi-functional Carbon cloths Condition Doped carbons Electrode performance Fluorine-doped Metal-oxide Neutral pH Overpotential Water electrolysis
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收录类别	EI ; SCI
语种	英语
资助项目	Vinnova, Sweden's Innovation Agency[DE210101259] ; null[2019-03174] ; null[2018-72190682]
WOS研究方向	Chemistry ; Energy & Fuels ; Materials Science
WOS类目	Chemistry, Physical ; Energy & Fuels ; Materials Science, Multidisciplinary
WOS记录号	WOS:000969281800001
出版者	Royal Society of Chemistry
EI入藏号	20231814031020
EI主题词	Pyridine
EI分类号	547.1 Precious Metals ; 802.2 Chemical Reactions ; 803 Chemical Agents and Basic Industrial Chemicals ; 804 Chemical Products Generally ; 804.1 Organic Compounds ; 931.3 Atomic and Molecular Physics
原始文献类型	Article in Press
引用统计
文献类型	期刊论文
条目标识符	https://kms.shanghaitech.edu.cn/handle/2MSLDSTB/299879
专题	物质科学与技术学院物质科学与技术学院_博士生大科学中心_PI研究组_翁祖谦组
通讯作者	Das, Biswanath; Verho, Oscar; Akermark, Bjorn
作者单位	1.Stockholm Univ, Dept Organ Chem, Arrhenius Lab, Svante Arrhenius Vag 16C, S-10691 Stockholm, Sweden 2.KTH Royal Inst Technol, Dept Appl Phys, Hannes Alfvens Vag 12, S-11419 Stockholm, Sweden 3.ShanghaiTech Univ, Sch Phys Sci & Technol, Shanghai 201210, Peoples R China 4.Stockholm Univ, Dept Mat & Environm Chem, Svante Arrhenius Vag 16C, S-10691 Stockholm, Sweden 5.Univ Wuppertal, Inorgan Chem, Gaussstr 20, D-42119 Wuppertal, Germany 6.KTH Royal Inst Technol, Mat & Nanophys, Hannes Alfvens Vag 12, S-11419 Stockholm, Sweden 7.Univ New South Wales, Sch Chem Engn, Sydney 2052, Australia 8.Uppsala Univ, Dept Med Chem, Biomed Ctr BMC, SE-75123 Uppsala, Sweden 9.KTH Royal Inst Technol, Dept Chem, SE-10044 Stockholm, Sweden
推荐引用方式 GB/T 7714	Das, Biswanath,Toledo-Carrillo, Esteban A.,Li, Guoqi,et al. Bifunctional and regenerable molecular electrode for water electrolysis at neutral pH[J]. JOURNAL OF MATERIALS CHEMISTRY A,2023,11(25):13331-13340.
APA	Das, Biswanath.,Toledo-Carrillo, Esteban A..,Li, Guoqi.,Stahle, Jonas.,Thersleff, Thomas.,...&Akermark, Bjorn.(2023).Bifunctional and regenerable molecular electrode for water electrolysis at neutral pH.JOURNAL OF MATERIALS CHEMISTRY A,11(25),13331-13340.
MLA	Das, Biswanath,et al."Bifunctional and regenerable molecular electrode for water electrolysis at neutral pH".JOURNAL OF MATERIALS CHEMISTRY A 11.25(2023):13331-13340.