Self-Reconstruction of Sulfate-Containing High Entropy Sulfide for Exceptionally High-Performance Oxygen Evolution Reaction Electrocatalyst
Self-Reconstruction of Sulfate-Containing High Entropy Sulfide for Exceptionally High-Performance Oxygen Evolution Reaction Electrocatalyst
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DOI：
10.1002/adfm.202106229
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发表时间：
2021-08-31
影响因子：
19
通讯作者：
Ting, Jyh-Ming
中科院分区：
文献类型：
--
作者：
Nguyen, Thi Xuyen;Su, Yen-Hsun;Ting, Jyh-Ming
通过两步溶剂热法合成了富含金属硫酸盐的新型高熵硫化物 FeNiCoCrXS2（其中 X = Mn、Cu、Zn 或 Al）。结果表明，含硫酸盐的 FeNiCoCrMnS2 表现出优异的析氧反应（OER）活性，在电流密度为 10、100、500 和 1000 mA cm(-2) 时，过电位分别为 199、246、285 和 308 mV，超过其一元、二元、三元和四元金属对应物。即使在 500 mA cm(-2) 的高电流密度下，该电催化剂在 12 000 次循环后仍具有出色的稳定性和 55 小时的耐久性。首次使用各种原位和非原位分析来研究 OER 期间硫化物的自重建。由此产生的金属（羟基）氢氧化物被认为是 OER 的真正活性中心。剩余的硫酸盐也有助于催化活性。密度函数理论计算与实验结果吻合较好。高熵硫化物非凡的OER性能为实际应用中理想的催化剂设计带来了绝佳的机会。
Novel earth-abundant metal sulfate-containing high entropy sulfides, FeNiCoCrXS2 (where X = Mn, Cu, Zn, or Al), are synthesized via a two-step solvothermal method. It is shown that sulfate-containing FeNiCoCrMnS2 exhibits superior oxygen evolution reaction (OER) activity with an exceptionally low overpotential of 199, 246, 285, and 308 mV at current densities of 10, 100, 500, and 1000 mA cm(-2), respectively, and surpassing its unary-, binary-, ternary-, and quaternary-metal counterparts. The electrocatalyst yields exceptional stability after 12 000 cycles and 55 h of durability even at a high current density of 500 mA cm(-2). Various in situ and ex situ analyses are used to investigate the self-reconstruction of the sulfides during the OER for the first time. The resulting metal (oxy)hydroxide is believed to be the true active center for OER. The remaining sulfate also contributes to the catalytic activity. Density function theory calculation is in good agreement with the experimental result. The extraordinary OER performance of the high entropy sulfide brings a great opportunity for desirable catalyst design for practical applications.