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Piezocatalytic pure water splitting for H2 evolution carries the virtues of efficacious utilization of mechanical energy, easy operation, and high value‐added products, while lacking desirable piezoelectrics for high chemical energy production. Here, two polar layered bismuth‐rich oxyhalides Bi4O5X2 (XBr, I) thin nanosheets (≈4 nm) are first exploited as efficient piezocatalysts to be capable of...
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