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Characterization of paramagnetic states in an organometallic nickel hydrogen evolution electrocatalyst
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Characterization of paramagnetic states in an organometallic nickel hydrogen evolution electrocatalyst
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Journal Article
Characterization of paramagnetic states in an organometallic nickel hydrogen evolution electrocatalyst
2023
Overview
Significant progress has been made in the bioinorganic modeling of the paramagnetic states believed to be involved in the hydrogen redox chemistry catalyzed by [NiFe] hydrogenase. However, the characterization and isolation of intermediates involved in mononuclear Ni electrocatalysts which are reported to operate through a Ni
I/III
cycle have largely remained elusive. Herein, we report a Ni
II
complex (NCHS2)Ni(OTf)2, where NCHS2 is 3,7-dithia-1(2,6)-pyridina-5(1,3)-benzenacyclooctaphane, that is an efficient electrocatalyst for the hydrogen evolution reaction (HER) with turnover frequencies of ~3,000 s
−1
and a overpotential of 670 mV in the presence of trifluoroacetic acid. This electrocatalyst follows a hitherto unobserved HER mechanism involving C-H activation, which manifests as an inverse kinetic isotope effect for the overall hydrogen evolution reaction, and Ni
I
/Ni
III
intermediates, which have been characterized by EPR spectroscopy. We further validate the possibility of the involvement of Ni
III
intermediates by the independent synthesis and characterization of organometallic Ni
III
complexes.
The characterization of nickel (Ni)‐centred paramagnetic states relevant to [NiFe] hydrogenases is rare in mononuclear Ni hydrogen evolution catalysts. Here, the authors report the spectroscopic and synthetic characterization of Ni
I
and Ni
III
states in an organometallic Ni hydrogen evolution catalyst.
Publisher
Nature Publishing Group UK,Nature Publishing Group,Nature Portfolio
