Trifunctional electrocatalysis for the oxygen evolution reaction, oxygen reduction reaction, and hydrogen evolution reaction constitutes the bottleneck of various sustainable energy devices and systems including rechargeable metal–air batteries and overall water splitting. Emerging macroscopically nanostructured catalysts are strongly requested for superior electrocatalytic activities and practical applications. Here, a 3D hydroxysulfide monolith with anion‐regulated NiFe hydroxysulfide nanosheets is rationally proposed. With abundant active sites and unique structure, the as‐obtained hydroxysulfide monolith exhibits superior electrocatalytic performance in oxygen evolution, hydrogen evolution, and oxygen reduction in alkaline electrolyte. When directly serving as electrodes, a small charge/discharge voltage gap of 0.76 V at 2.0 mA cm⁻² and a high peak power density of 248 mW cm⁻² are achieved for the liquid Zn−air batteries, and a low cell voltage of 1.62 V at 10 mA cm⁻² is detected for water splitting units. When two Zn−air batteries are serially connected to power the water splitting unit, bulky O₂ and H₂ bubbles are continuously generated on both the composite electrodes. This work demonstrates an effective strategy for controllable anion regulation and rational design of the 3D self‐supporting hydroxysulfides, which is also enlightening for other advanced energy materials and diverse applications.

中文翻译：

---

阴离子调控的羟基硫化物整体材料作为OER / ORR / HER电催化剂及其在自供电式电化学水分解中的应用

氧气释放反应，氧气还原反应和氢气释放反应的三功能电催化反应构成了各种可持续能源设备和系统的瓶颈，包括可充电金属-空气电池和总水分解。对于优异的电催化活性和实际应用，强烈要求使用新兴的宏观纳米结构催化剂。在这里，合理地提出了带有阴离子调节的NiFe羟基硫化物纳米片的3D羟基硫化物整体结构。如此获得的羟基硫化物整体物具有丰富的活性位点和独特的结构，在碱性电解液中的氧气释放，氢气释放和氧气还原方面表现出优异的电催化性能。直接用作电极时，在2.0 mA cm处有0.76 V的小充电/放电电压间隙对于液态Zn-空气电池，实现了^-2和248 mW cm ^-2的高峰值功率密度，并且对于水分解单元，在10 mA cm ^-2处检测到了1.62 V的低电池电压。当两个Zn-air电池串联连接以为分水单元供电时，两个复合电极上都会连续产生大体积的O ₂和H ₂气泡。这项工作展示了一种可控的阴离子调节和3D自支撑羟基硫化物合理设计的有效策略，这对于其他先进的能源材料和各种应用也具有启发性。