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101 0 _aeng
135 _adrcn ---uucaa
181 0 _ai
182 0 _ab
200 1 _aA Robust Molecular Catalyst Generated In?Situ for Photo- and Electrochemical Water Oxidation
_fH. A. Yo. Hassan [et al.]
203 _aText
_celectronic
300 _aTitle screen
320 _a[References: 56 tit.]
330 _aWater splitting is the key step towards artificial photosystems for solar energy conversion and storage in the form of chemical bonding. The oxidation of water is the bottle-neck of this process that hampers its practical utility; hence, efficient, robust, and easy to make catalytic systems based on cheap and earth-abundant materials are of exceptional importance. Herein, an in?situ generated cobalt catalyst, [CoII(TCA)2(H2O)2] (TCA=1-mesityl-1,2,3-1H-triazole-4-carboxylate), that efficiently conducts photochemical water oxidation under near-neutral conditions is presented. The catalyst showed high stability under photolytic conditions for more than 3?h of photoirradiation. During electrochemical water oxidation, the catalytic system assembled a catalyst film, which proved not to be cobalt oxide/hydroxide as normally expected, but instead, and for the first time, generated a molecular cobalt complex that incorporated the organic ligand bound to cobalt ions. The catalyst film exhibited a low overpotential for electrocatalytic water oxidation (360?mV) and high oxygen evolution peak current densities of 9 and 2.7?mA?cm?2 on glassy carbon and indium-doped tin oxide electrodes, respectively, at only 1.49 and 1.39?V (versus a normal hydrogen electrode), respectively, under neutral conditions. This finding, exemplified on the in?situ generated cobalt complex, might be applicable to other molecular systems and suggests that the formation of a catalytic film in electrochemical water oxidation experiments is not always an indication of catalyst decomposition and the formation of nanoparticles.
461 _tChemSusChem
463 _tVol. 10, iss. 5
_v[P. 862-875]
_d2017
610 1 _aэлектронный ресурс
610 1 _aтруды учёных ТПУ
610 1 _aмолекулярные компоненты
610 1 _aкатализаторы
610 1 _aфотоокисление
610 1 _aэлектрохимическое окисление
701 1 _aHassan
_bH. A. Yo.
_cchemical engineer
_cassistant of Tomsk Polytechnic University
_f1985-
_gHussein Abdelazeem Younus
_2stltpush
_3(RuTPU)RU\TPU\pers\39720
701 1 _aAhmad
_bN.
_cchemical engineer
_cassistant of Tomsk Polytechnic University
_f1981-
_gNazir
_2stltpush
_3(RuTPU)RU\TPU\pers\39722
701 1 _aChughtai
_bA. H.
_gAdeel
701 1 _aVandichel
_bM.
_gMatthias
701 1 _aBusch
_bM.
_gMichael
701 1 _aVan
_bH. K.
_gHecke Kristof
701 1 _aYusubov
_bM. S.
_cchemist
_cProfessor of Tomsk Polytechnic University, Doctor of chemical sciences
_f1961-
_gMekhman Suleiman-Ogly (Suleimanovich)
_2stltpush
_3(RuTPU)RU\TPU\pers\31833
701 1 _aSong
_bSh.
_gShaoxian
701 1 _aVerpoort
_bF. V. K.
_cChemical Engineer
_cProfessor of Tomsk Polytechnic University, doctor of chemical Sciences
_f1963-
_gFrensis Valter Kornelius
_2stltpush
_3(RuTPU)RU\TPU\pers\35059
712 0 2 _aНациональный исследовательский Томский политехнический университет (ТПУ)
_bИнститут природных ресурсов (ИПР)
_bКафедра технологии органических веществ и полимерных материалов (ТОВПМ)
_h6832
_2stltpush
_3(RuTPU)RU\TPU\col\18659
801 2 _aRU
_b63413507
_c20171027
_gRCR
856 4 _uhttp://dx.doi.org/10.1002/cssc.201601477
942 _cCF