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The catalytic hydrogen‐evolving activities of transition‐metal phosphides are greatly related to the phosphorus content, but the physical origin of performance enhancement remains ambiguous, and tuning the catalytic activity of nickel phosphides (NiP2/Ni5P4) remains challenging due to unfavorable H* adsorption. Here, a strategy is introduced to integrate P‐rich NiP2 and P‐poor Ni5P4 into in‐plane...
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