Developing low‐cost, highly active, and stable bifunctional electrocatalysts is a challenging issue in electrochemical water electrolysis. Building on 3D architectured electrocatalysts through structural and compositional engineering is an effective strategy to enhance catalytic activities as well as stability and durability. Herein, 3D architectures of quaternary Co‐Ni‐S‐P compounds coupled with graphene ((Co_1−xNi_x)(S_1−yP_y)₂/G) electrocatalysts are proposed, in which nanosheets are self‐assembled to form 3D architectures with round and flat doughnut‐like shapes, toward overall water splitting. Benefiting from the 3D architectures and Ni, P substitution, (Co_1−xNi_x)(S_1−yP_y)₂/G exhibits superior electrocatalytic activities with low overpotentials of 117 and 285 mV at 10 mA cm⁻² and Tafel slopes of 85 and 105 mV dec⁻¹ for hydrogen and oxygen evolution reactions, respectively, in alkaline media. In addition, minimal increases in overpotential are observed, even after the 10 000th voltammetric cycle and continuous chronopotentiometric testing over 50–100 h, confirming the high stability and durability of (Co_1−xNi_x)(S_1−yP_y)₂/G. When used as both cathode and anode, (Co_1−xNi_x)(S_1−yP_y)₂/G achieves excellent overall water splitting performance with a cell potential as low as 1.65 V, reaching a current density of 10 mA cm⁻² with no obvious decay after 50 h, demonstrating that (Co_1−xNi_x)(S_1−yP_y)₂/G is an efficient bifunctional electrocatalyst for overall water splitting.

中文翻译：

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第四级Co-Ni-S-P /石墨烯杂化物的3D体系结构作为高活性和稳定的双功能电催化剂，可用于总水分解

在电化学水电解中，开发低成本，高活性和稳定的双功能电催化剂是一个具有挑战性的问题。通过结构和组成工程在3D结构化的电催化剂上构建是提高催化活性以及稳定性和耐用性的有效策略。本文提出了季铵化Co-Ni-S-P化合物与石墨烯（（Co _{1- x} Ni _x）（S _{1- y} P _y）₂ / G）电催化剂的3D结构，其中纳米片被自组装成形成具有圆形和扁平甜甜圈形状的3D架构，以实现整体水分解。受益于3D架构和Ni，P替代，（Co _1-x Ni _x）（S _{1- y} P _y） ₂ / G表现出优异的电催化活性，在10 mA cm ^-2时低过电位为117和285 mV，对于氢和氧的释放反应的Tafel斜率分别为85和105 mV dec ^-1分别在碱性介质中。此外，即使在第10 000次伏安循环和连续计时电位测试超过50–100 h后，也观察到过小的电势增加，证实了（Co _{1- x} Ni _x）（S _{1- y} P _y）的高稳定性和耐用性。 _2个/G。当同时用作阴极和阳极时，（Co _{1- x} Ni _x）（S _{1- y} P _y）₂ / G可实现出色的整体水分解性能，电池电势低至1.65 V，电流密度达到10 mA cm ^-2在50 h后无明显衰减，表明（Co _{1- x} Ni _x）（S _{1- y} P _y）₂ / G是一种有效的双功能电催化剂，可用于总水分解。