Photochemical H 2 Evolution from Bis(diphosphine)nickel Hydrides Enables Low-Overpotential Electrocatalysis.

التفاصيل البيبلوغرافية
العنوان:	Photochemical H 2 Evolution from Bis(diphosphine)nickel Hydrides Enables Low-Overpotential Electrocatalysis.
المؤلفون:	Stratakes BM; Department of Chemistry, University of North Carolina at Chapel Hill, Chapel Hill, North Carolina 27599-3290, United States., Wells KA; Department of Chemistry, North Carolina State University, Raleigh, North Carolina 27695-8204, United States., Kurtz DA; Department of Chemistry, University of North Carolina at Chapel Hill, Chapel Hill, North Carolina 27599-3290, United States., Castellano FN; Department of Chemistry, North Carolina State University, Raleigh, North Carolina 27695-8204, United States., Miller AJM; Department of Chemistry, University of North Carolina at Chapel Hill, Chapel Hill, North Carolina 27599-3290, United States.
المصدر:	Journal of the American Chemical Society [J Am Chem Soc] 2021 Dec 22; Vol. 143 (50), pp. 21388-21401. Date of Electronic Publication: 2021 Dec 08.
نوع المنشور:	Journal Article; Research Support, U.S. Gov't, Non-P.H.S.
اللغة:	English
بيانات الدورية:	Publisher: American Chemical Society Country of Publication: United States NLM ID: 7503056 Publication Model: Print-Electronic Cited Medium: Internet ISSN: 1520-5126 (Electronic) Linking ISSN: 00027863 NLM ISO Abbreviation: J Am Chem Soc Subsets: PubMed not MEDLINE; MEDLINE
أسماء مطبوعة:	Publication: Washington, DC : American Chemical Society Original Publication: Easton, Pa. [etc.]
مستخلص:	Molecules capable of both harvesting light and forming new chemical bonds hold promise for applications in the generation of solar fuels, but such first-row transition metal photoelectrocatalysts are lacking. Here we report nickel photoelectrocatalysts for H 2 evolution, leveraging visible-light-driven photochemical H 2 evolution from bis(diphosphine)nickel hydride complexes. A suite of experimental and theoretical analyses, including time-resolved spectroscopy and continuous irradiation quantum yield measurements, led to a proposed mechanism of H 2 evolution involving a short-lived singlet excited state that undergoes homolysis of the Ni-H bond. Thermodynamic analyses provide a basis for understanding and predicting the observed photoelectrocatalytic H 2 evolution by a 3d transition metal based catalyst. Of particular note is the dramatic change in the electrochemical overpotential: in the dark, the nickel complexes require strong acids and therefore high overpotentials for electrocatalysis; but under illumination, the use of weaker acids at the same applied potential results in a more than 500 mV improvement in electrochemical overpotential. New insight into first-row transition metal hydride photochemistry thus enables photoelectrocatalytic H 2 evolution without electrochemical overpotential (at the thermodynamic potential or 0 mV overpotential). This catalyst system does not require sacrificial chemical reductants or light-harvesting semiconductor materials and produces H 2 at rates similar to molecular catalysts attached to silicon.
تواريخ الأحداث:	Date Created: 20211208 Date Completed: 20220203 Latest Revision: 20220203
رمز التحديث:	20231215
DOI:	10.1021/jacs.1c10628
PMID:	34878278
قاعدة البيانات:	MEDLINE

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الوصف
تدمد:	1520-5126
DOI:	10.1021/jacs.1c10628