Huang Huajie, Xiao Di, Zhu Zihan, Zhang Chi, Yang Lu, He Haiyan, You Jungmok, Jiang Quanguo, Xu Xingtao, Yamauchi Yusuke
College of Mechanics and Materials, Hohai University Nanjing 210098 China
Department of Plant & Environmental New Resources, College of Life Sciences, Kyung Hee University 1732 Deogyeong-daero, Giheung-gu Yongin-si Gyeonggi-do 17104 South Korea.
Chem Sci. 2023 Sep 4;14(36):9854-9862. doi: 10.1039/d3sc03735e. eCollection 2023 Sep 20.
Two-dimensional (2D) Pd nanosheet-based catalysts have recently garnered widespread attention due to their high atom utilization efficiency. However, their catalytic ability and structural stability still require significant enhancement before they can be widely applied. In this study, we presented the rational design and controllable fabrication of a novel 2D/2D heterojunction, which consists of ultrathin Pd nanosheets (NSs) grown on the TiCT MXene surface (Pd NSs/MXene). This heterostructure was achieved through a robust and convenient stereo-assembly strategy. The newly developed Pd NSs/MXene heterojunction not only provides numerous exposed active Pd atoms with an optimized electronic structure but also enables an intimate Pd/MXene interfacial interaction, ensuring a stable hybrid configuration. Consequently, the resulting Pd NSs/MXene heterojunction exhibits exceptional methanol oxidation properties. It possesses a large electrochemically active surface area, high mass and specific activities, and a long operating life, which are significantly superior to those of traditional Pd nanoparticle/carbon and Pd nanosheet/carbon catalysts. Theoretical simulations further reveal strong electronic interactions between the Pd nanosheet and MXene, which dramatically enhance the adsorption energy of the Pd component and simultaneously lower its d-band center. As a result, the Pd NSs/MXene heterojunction is less susceptible to CO poisoning. This work introduces a new 2D/2D heterojunction based on MXene and noble metallic materials and holds significance for the development of other novel heterojunctions, particularly within the realm of 2D material nanoarchitectonics.
基于二维(2D)钯纳米片的催化剂近来因其高原子利用效率而受到广泛关注。然而,在其能够被广泛应用之前,它们的催化能力和结构稳定性仍需要显著提高。在本研究中,我们展示了一种新型二维/二维异质结的合理设计与可控制备,该异质结由生长在TiCT MXene表面的超薄钯纳米片(NSs)组成(钯纳米片/ MXene)。这种异质结构是通过一种稳健且便捷的立体组装策略实现的。新开发的钯纳米片/ MXene异质结不仅提供了大量具有优化电子结构的暴露活性钯原子,还实现了紧密的钯/ MXene界面相互作用,确保了稳定的混合结构。因此,所得的钯纳米片/ MXene异质结表现出优异的甲醇氧化性能。它具有大的电化学活性表面积、高质量比活性和比活性以及长的使用寿命,显著优于传统的钯纳米颗粒/碳和钯纳米片/碳催化剂。理论模拟进一步揭示了钯纳米片与MXene之间强烈的电子相互作用,这极大地提高了钯组分的吸附能,同时降低了其d带中心。结果,钯纳米片/ MXene异质结对CO中毒的敏感性较低。这项工作引入了一种基于MXene和贵金属材料的新型二维/二维异质结,对其他新型异质结的开发具有重要意义,特别是在二维材料纳米结构领域。