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2D/2D heterojunction interface: Engineering of 1T/2H MoS2 coupled with Ti3C2Tx heterostructured electrocatalysts for pH-universal hydrogen evolution
Journal of Materials Science & Technology ( IF 11.2 ) Pub Date : 2023-10-18 , DOI: 10.1016/j.jmst.2023.10.002
Jian Yiing Loh , Feng Ming Yap , Wee-Jun Ong

Two-dimensional (2D) materials have come to light due to their unique thickness that owns abundant exposed edges with enhanced electrocatalytic properties. 2D molybdenum disulfide (MoS2) nanosheet has aroused considerable attention due to its tunable surface chemistry and high electrochemical surface area. Nonetheless, several shortcomings associated with MoS2, such as its naturally existing semiconducting 2H phase, which has limited active sites due to the inert basal plane, restrict its application in water electrocatalysis. Taking into account the benefits of the 1T/2H phase of MoS2, as well as the importance of engineering 2D/2D heterojunction interface for boosted electrocatalysis, metallic Ti3C2Tx was integrated with 1T/2H MoS2 to develop 2D/2D 1T/2H MoS2/Ti3C2Tx heterostructured nanocomposites. Herein, with only 25% of the intercalating agent, 1T/2H MoS2 with the highest 1T phase content of ∼82% was successfully synthesized. It was further incorporated with 1 wt% of Ti3C2Tx through a combination of ultrasonication and mechanical stirring process. The 1T/2H MoS2 (25D)/ Ti3C2Tx-1 (MTC-1) manifested outstanding electrocatalytic performance with an overpotential and Tafel slope of 280 mV (83.80 mV dec–1) and 300 mV (117.2 mV dec–1), for catalyzing acidic and alkaline medium HER, respectively. Pivotally, the as-prepared catalysts also illustrated long-term stability for more than 40 h. The coupling method for the 2D nanosheets is crucial to suppress the oxidation of Ti3C2Tx and the restacking issue of 2D nanosheets. The superior HER activity is ascribed to the synergistic effect between the heterostructure, enhancing the electronic structure and charge separation capability. The intrinsic property of the catalyst further confirms by turnover frequency (TOF) calculation. As such, this research paves the way for designing high-efficiency 2D electrocatalysts and sheds light on the further advancement of tunable 2D electrocatalysts for robust water splitting and beyond.



中文翻译:

2D/2D 异质结界面:1T/2H MoS2 与 Ti3C2TX 异质结电催化剂相结合的工程设计,用于 pH 通用析氢

二维(2D)材料因其独特的厚度而闻名,该材料具有丰富的暴露边缘和增强的电催化性能。二维二硫化钼(MoS2 纳米片由于其可调节的表面化学性质和高电化学表面积而引起了广泛的关注。尽管如此,与MoS 2相关的几个缺点,例如其天然存在的半导体2H相,由于惰性基面而具有有限的活性位点,限制了其在水电催化中的应用。考虑到MoS 2 1T/2H相的优点,以及设计2D/2D异质结界面对于增强电催化的重要性,将金属Ti 3 C 2 T x与1T/2H MoS 2集成以开发2D/ 2D 1T/2H MoS 2 /Ti 3 C 2 T x异质结构纳米复合材料。在此,仅用25%的插层剂,就成功合成了最高1T相含量~82%的1T/2H MoS 2 。通过超声波处理和机械搅拌工艺的结合,进一步掺入1wt%的Ti 3 C 2 T x 。1T/2H MoS 2 (25D)/ Ti 3 C 2 T x -1 (MTC-1) 表现出出色的电催化性能,过电势和塔菲尔斜率分别为 280 mV (83.80 mV dec –1 ) 和 300 mV (117.2 mV dec) –1 ),分别用于催化酸性和碱性介质 HER。关键的是,所制备的催化剂还表现出超过 40 小时的长期稳定性。二维纳米片的耦合方法对于抑制Ti 3 C 2 T x的氧化和二维纳米片的重新堆叠问题至关重要。优异的HER活性归因于异质结构之间的协同效应,增强了电子结构和电荷分离能力。通过周转频率(TOF)计算进一步证实了催化剂的内在性质。因此,这项研究为设计高效二维电催化剂铺平了道路,并揭示了可调谐二维电催化剂的进一步发展,以实现稳健的水分解等。

更新日期:2023-10-18
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