Dyes and Pigments ( IF 4.1 ) Pub Date : 2022-08-07 , DOI: 10.1016/j.dyepig.2022.110620
Aijian Wang , Qi Wang , Yuqin Dou , M. Shire Sudi , Weihua Zhu , Danhong Shang , Longhua Li
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The electrochemical water splitting in strongly acidic medium with noble-metal-free electrocatalysts remains a desirable yet technological challenge. Herein, we developed a series of porphyrin coordination polymer supported transition-metal sulfides as bifunctional electrocatalysts (Co3S4@MoS2@nTiPCP, n = 10, 20 or 30) that performs well in acidic media. The optimal Co3S4@MoS2@20TiPCP achieves current densities of 10 mA cm−2 at overpotentials of 247 and 110 mV for acidic OER and HER, respectively. Particularly, an electrolyzer with better long-term stability using Co3S4@MoS2@20TiPCP as both cathode and anode exhibits a low cell voltage of 1.41 V at 10 mA cm−2 in acid, outperforming most other reported electrocatalysts elsewhere. The efficient electrochemical water splitting is ascribed to the synergetic effect and the unique structure characteristics. DFT calculations demonstrate that the Co atoms in Co3S4@MoS2@20TiPCP are the major active sites for electrochemical water splitting thanks to regulated electronic structures and reduced reaction energy barrier.
中文翻译:

卟啉配位聚合物负载的过渡金属硫化物作为无贵金属电催化剂用于高效的整体水分解
具有无贵金属电催化剂的强酸性介质中的电化学水分解仍然是一个理想的技术挑战。在此,我们开发了一系列卟啉配位聚合物负载的过渡金属硫化物作为双功能电催化剂(Co 3 S 4 @MoS 2 @nTiPCP,n = 10、20 或 30),在酸性介质中表现良好。最佳的 Co 3 S 4 @MoS 2 @20TiPCP在酸性 OER和 HER的过电势分别为 247 和 110 mV 时实现了 10 mA cm -2的电流密度。特别是使用 Co 3 S的电解槽具有更好的长期稳定性4 @MoS 2 @20TiPCP 作为阴极和阳极,在 10 mA cm -2酸中表现出 1.41 V 的低电池电压,优于其他地方报道的大多数其他电催化剂。高效的电化学水分解归因于协同效应和独特的结构特征。DFT 计算表明,由于电子结构可控和反应能垒降低,Co 3 S 4 @MoS 2 @20TiPCP 中的 Co 原子是电化学水分解的主要活性位点。