Abstract

In realizing clean and viable electrochemical technologies for chemical conversions or energy storage, it is of utmost importance to develop economical and high-performance electrode materials. Transition metal dichalcogenides (TMDs), in particular, are attractive candidates on account of their exceptional physicochemical properties. To further enhance their performances, the construction of TMD-based heterostructures has been identified to yield a new class of promising materials with enhanced functionality, stability, and efficiencies, even surpassing that of noble metal benchmarks. In this review, we highlight recent progress in the development of TMD-based heterostructures for electrocatalytic conversion systems (hydrogen evolution reaction) and electrochemical energy-storage systems (LiB/NiB/supercapacitors). Vital strategies for rational design of these heterostructures are discussed, and future directions in overcoming key limitations are provided. We hope that the perspectives presented will facilitate advancements in attaining new and improved TMD-based heterostructures better suited for the respective applications. Transition metal dichalcogenides (TMDs) are promising materials for use in electrocatalytic and electrochemical energy-storage systems owing to their exceptional physicochemical properties, including large surface area, remarkable mechanical properties, high catalytic activity, chemical stability, and low cost. In further improving material properties tailored to meet application-specific requirements, heterostructure construction holds significant advantages, benefiting from the synergistic effect between constituents involved. TMD-based heterostructures have been widely explored recently, giving rise to diverse materials with desirable characteristics such as significantly increased interfacial contact of low resistance for efficient electron transfers, constituent-dependent electronic structure, tunable layer distances facilitating easily intercalation of redox species, and increased surface area for effective interaction with electrolyte. In this review, TMD-based heterostructures are assessed for performance in electrocatalytic conversion (hydrogen evolution reaction) and electrochemical energy-storage systems (NiB/LiB/supercapacitors). The impactful strategies employed in overcoming key challenges are evaluated, and finally, future directions for TMD-based heterostructure construction are presented. Transition metal dichalcogenides (TMDs) are promising materials for use in electrocatalytic and electrochemical energy-storage systems owing to their exceptional physicochemical properties, including large surface area, remarkable mechanical properties, high catalytic activity, chemical stability, and low cost. In further improving material properties tailored to meet application-specific requirements, heterostructure construction holds significant advantages, benefiting from the synergistic effect between constituents involved. TMD-based heterostructures have been widely explored recently, giving rise to diverse materials with desirable characteristics such as significantly increased interfacial contact of low resistance for efficient electron transfers, constituent-dependent electronic structure, tunable layer distances facilitating easily intercalation of redox species, and increased surface area for effective interaction with electrolyte. In this review, TMD-based heterostructures are assessed for performance in electrocatalytic conversion (hydrogen evolution reaction) and electrochemical energy-storage systems (NiB/LiB/supercapacitors). The impactful strategies employed in overcoming key challenges are evaluated, and finally, future directions for TMD-based heterostructure construction are presented. The constant pursuit for development and modernization necessitates extensive and ever-increasing global energy consumption, imposing strain on our current availability of non-renewable fossil fuel resources and raising concern about eventual depletion.1Chu S. Majumdar A. Opportunities and challenges for a sustainable energy future.Nature. 2012; 488: 294-303Crossref PubMed Scopus (3049) Google Scholar,2Jeffrey C. Raymond J.K. Paul R.P. 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Considering this challenge in attaining superior electrochemical performance, the careful selection and combination of multiple solid-state materials into formation of heterostructures has become an appealing concept for the associated constituents to institute an advantageous synergistic effect that endows the material with enhanced and favorable physicochemical properties tailored to satisfy the application-specific requirements.10Gnanasekar P. Periyanagounder D. Kulandaivel J. Vertically aligned MoS2 nanosheets on graphene for highly stable electrocatalytic hydrogen evolution reactions.Nanoscale. 2019; 11: 2439-2446Crossref PubMed Google Scholar In particular, design and fabrication of active heterostructure electrodes involving nanomaterials is appealing. On the basis of dimensions, the nanomaterial constituents may be classified into 0D, which comprises nanoparticles or quantum dots, 1D, as in nanowires or nanotubes, and lastly, 2D layered nanomaterials such as nanosheets (NSs) and nanoflakes. Among these, the 2D layered nanomaterials are typically prospective candidates for the fabrication of heterostructure electrodes on account of their unique and remarkable structural properties, having atomic-layer thickness and largest exposed surface area, effectuating the greatest surface redox reactions.11Yun Q. Li L. Hu Z. Lu Q. Chen B. Zhang H. Layered transition metal dichalcogenide-based nanomaterials for electrochemical energy storage.Adv. Mater. 2019; 32: 1903826Crossref Scopus (2) Google Scholar Furthermore, since the advent of graphene in 2004, a wide spectrum of 2D nanomaterials has been developed for consideration, including transition metal dichalcogenides (TMDs), MXenes, halides, oxides, and hydroxides, among others.12Geim A.K. 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Here, we present a critical review of recent developments, discussing the latest impactful work concerning TMD-based heterostructures, taking into account specific examples of electrocatalytic conversion systems (hydrogen evolution reaction [HER]) and electrochemical energy-storage systems (Li-ion batteries [LiB]/Na-ion batteries [NiB]/supercapacitors). Strategies employed in the rational design of these materials are discussed. Finally, the challenges ahead and directions for future TMD-based heterostructure construction are presented. As discussed previously, electrochemical approaches are seemingly advantageous solutions, offering a means to harness intermittent but renewable energy sources (i.e., solar energy) for electricity generation, which in turn can be channeled through electrocatalytic conversion technologies for a clean and sustainable means of driving chemical conversions into fuel resources.4Laursen A.B. Dahl S. Chorkendorff I. Kegnæs S. 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Mater. 2015; 25: 6199-6204Crossref Scopus (64) Google Scholar On the other hand, the edge sites predominantly contribute as catalytically active sites, driving transformations to adsorbed species through electron transfers and redox processes. In this regard, the fraction of edge to basal sites holds direct correlation with HER activity. Besides the renowned strategies of employing low-dimensional nanomaterials (0D, 1D, 2D) and reducing their size dimensions further, several other key techniques have been explored to increase fraction and exposure of edge sites for superior HER performance, such as designing suitable architectures and engineering of defects.61Ouyang Y. Ling C. Chen Q. Wang Z. Shi L. Wang J. Activating inert basal planes

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