Heterogeneous Water Splitting Catalysts


Our recent works on solid catalysts for the oxygen evolution/reduction reactions (OER/ORR) are focused on 3d transition metals as a common thread. We proceed to embed and analyze them into a variety of 3D environments. A strong emphasis is placed from the beginning on the fascinating interplay of preparative methods, resulting in properties and performance of oxide OER catalysts, such as in Co-spinels (Chem. Eur. J. 2018, 24, 18242; ACS Omega 2019, 4, 15444), or recently in Mn-oxides (ACS Catal. 2020, 10, 2074; ACS Catal. 2021, 11, 5, 2511–2523).


ACS Catal. 2021, 11, 5, 2511–2523

This line of research is complemented by operando OER and analytical studies of transition metal carbodiimide (MNCN) systems, which consist of catalytic centers confined within uniquely well-defined all-nitrogen {MN6} moieties (Dalton Trans. 2018, 47, 10759; Anal. Chem. 2018, 90, 9234). Recently, we also explored the nanoscale morphology control of 3d transition metal centers in N/C- and sulfur matrices, bringing forward Co/Fe/Ni-sulfide nanoboxes with robust bifunctional OER/HER electrocatalytic properties (Chem. Mater. 2020, 32, 1371). Through engineering reduced Ni/Fe-ultrathin coordination polymers from cyanometallate precursors, we revealed new mechanistic insights into their Ni-O-Fe dual active sites (Adv. Energy Mater. 2020, 2002228).


ACS Nano 2020 (14) 13279

These works inspired us to enter the dynamic field of single-atom catalysts (SACs) by using a facile approach for the soft-landing of well-defined Co/Ni/Fe-phthalocyanines on graphene oxide, followed by operando and computational insight into their dual OER/ORR pathways as a function of the metal center and coordination environment (ACS Nano 2020 (14) 13279).

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