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High-performance hydrogen evolution reaction (HER) catalysts are compelling for the conversion of renewable electricity to fuels and feedstocks. The best HER catalysts rely on the use of platinum and show the highest performance in acidic media. Efficient HER catalysts based on inexpensive and Earth-abundant elements that operate in neutral (hence biocompatible) media could enable low-cost direct seawater splitting and the realization of bio-upgraded chemical fuels. In the challenging neutral-pH environment, water splitting is a multistep reaction. Here we present a HER catalyst comprising Ni and CrO_x sites doped onto a Cu surface that operates efficiently in neutral media. The Ni and CrO_x sites have strong binding energies for hydrogen and hydroxyl groups, respectively, which accelerates water dissociation, whereas the Cu has a weak hydrogen binding energy, promoting hydride coupling. The resulting …