期刊
ACS NANO
卷 17, 期 17, 页码 17254-17264出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsnano.3c05224
关键词
metal-organic frameworks; phosphorene; bond polarizability; water oxidation; electrocatalysis; lattice oxygen mechanism
A Ni metal-organic framework/black phosphorene heterostructure is used to optimize the performance of oxygen evolution reaction (OER). The p-type black phosphorene host increases the Ni-O bond polarizability of NiMOF, allowing for enhanced LOM pathway and OER performance. Experimental and computational results demonstrate the activated LOM pathway with a more balanced step barrier in the NiMOF/BP OER catalyst.
The emerging lattice-oxygen oxidation mechanism (LOM) presents attractive opportunities for breaking the scaling relationship to boost oxygen evolution reaction (OER) with the direct O-Lattice*O interaction. However, currently the LOM-triggering rationales are still debated, and a streamlined physicochemical paradigm is extremely desirable for the design of LOM-defined OER catalysts. Herein, a Ni metal-organic framework/black phosphorene (NiMOF/BP) heterostructure is theoretically profiled and constructed as a catalytic platform for the LOM-derived OER studies. It is found that the p-type BP host can enlarge the Ni-O bond polarizability of NiMOF through the Ni-O bond stretching and Ni valence declining synergically. Such an enlarged bond polarizability will in principle alleviate the lattice oxygen confinement to benefit the LOM pathway and OER performance. As a result, the optimized NiMOF/BP catalyst exhibits promising OER performance with a low overpotential of 260 mV at 10 mA cm(-2) and long-term stability in 1 M KOH electrolyte. Both experiment and calculation results suggest the activated LOM pathway with a more balanced step barrier in the NiMOF/BP OER catalyst. This research puts forward Ni-O bond polarizability as the criterion to design LOM-scaled electrocatalysts for water oxidation.
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