Chen, Ying-YuYing-YuChenKubendhiran, SubbiramaniyanSubbiramaniyanKubendhiranPerumal, SakthivelSakthivelPerumalLee, Pin-YanPin-YanLeeLin, Shan-NiShan-NiLinWen-Yueh YuLin, Lu-YinLu-YinLinKUO-CHUAN HO2026-03-242026-03-242026-04https://www.scopus.com/record/display.uri?eid=2-s2.0-105029678351&origin=resultslisthttps://scholars.lib.ntu.edu.tw/handle/123456789/736622In this work, a high-entropy MOF-74 precursor containing Fe, Co, Mn, and Mo is in situ grown on nickel foam, providing a well-integrated and conductive framework. The precursor is then carbonized under an Ar/H2 atmosphere, which partially reduces the multimetal centers to their zero-valent states, and subsequently sulfurization via chemical vapor deposition to yield a high-entropy MOF-derived metal sulfide (FeCoMnMo/NF-C-S). This sequential structural evolution leads to entropy-stabilized reconstruction, enhanced electrical conductivity, and a defect-rich surface, collectively lowering the overpotentials at each stage of synthesis. The resulting FeCoMnMo/NF-C-S demonstrates exceptional electrocatalytic performance, requiring only 36 mV for HER and 174 mV for OER at 10 mA cm−2. High current densities of 1000 mA cm−2 are achieved at overpotentials of just 295 and 309 mV for HER and OER, respectively. In a two-electrode configuration, cell voltages of 1.45 and 2.00 V enable 10 and 1000 mA cm−2. The catalyst also maintains stable operation for 120 h under both low and high current densities, confirming its bifunctional efficiency and durability. This study introduces an in-situ growth and entropy-engineered transformation strategy that integrates high-entropy chemistry with MOF-derived flower-like nanostructures, enabling a uniquely efficient and durable bifunctional catalyst for overall water splitting.falseElectrocatalytic water splittingHigh-entropy metal sulfidesHydrogen evolution reactionMetal organic frameworkOverall water splittingOxygen evolution reactionjournal article10.1016/j.mtener.2026.1022262-s2.0-105029678351