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Highly effective photocatalysts for the hydrogen‐evolution reaction were developed by conferring the linkers of NH2‐MIL‐125(Ti), a metal–organic framework (MOF) constructed from TiOx clusters and 2‐aminoterephthalic acid (linkers), with active copper centers. This design enables effective transfer of electrons from the linkers to the transient Cu2+/Cu+ centers, leading to 7000‐fold and 27‐fold increase...
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