Inducing the rapid and deep self-reconstruction of anodes has the potential to achieve the desired structure for effective oxygen evolution reactions (OERs) in seawater, but it is challenging. Herein, sulfur-assisted structural reconstruction of transition metal molybdates was fabricated. Benefiting from the electronic escape effect that occurs due to metal–O/–S bonding orbitals in the pre-catalyst, deep electrochemical reconstruction to highly active S-doped oxyhydroxides was achieved via rational S–metal hybridization and phase transition in the pre-catalyst. Meanwhile, combining the theoretical calculations and spectroscopic tests, it was found that introducing S atoms into oxyhydroxides activated lattice oxygen atoms, thereby boosting the intrinsic OER activity following the lattice oxygen mechanism pathway. As tested, the final S-doped oxyhydroxide catalysts exhibited excellent electrocatalytic activity with an ultralow overpotential of 166 mV at 10 mA cm−2 in alkaline seawater oxidation. This work showcased a feasible strategy of sulfur-assisted structural reconstruction to fabricate highly efficient and chemically stable materials for seawater splitting.

中文翻译：

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硫促进过渡金属钼酸盐的原位深层重建，实现碱性海水的卓越电催化氧化


诱导阳极的快速和深度自重构有可能实现海水中有效析氧反应 （OER） 所需的结构，但具有挑战性。在此，制备了过渡金属钼酸盐的硫辅助结构重建。受益于预催化剂中金属-O/-S 键合轨道产生的电子逃逸效应，通过在预催化剂中实现合理的 S-金属杂化和相变，实现了对高活性 S 掺杂羟基氧化物的深度电化学重构。同时，结合理论计算和光谱测试，发现将 S 原子引入氢氧化物中会激活晶格氧原子，从而促进遵循晶格氧机制途径的本征 OER 活性。经测试，最终的 S 掺杂氢氧化物催化剂表现出优异的电催化活性，在碱性海水氧化中，在 10 mA cm-2 处具有 166 mV 的超低过电位。这项工作展示了一种可行的硫辅助结构重建策略，以制备高效且化学稳定的海水分解材料。