Electro-, photo-, and photoelectrocatalysis play a critical role toward the realization of a sustainable energy economy. They facilitate numerous redox reactions in energy storage and conversion systems, enabling the production of chemical feedstock and clean fuels from abundant resources like water, carbon dioxide, and nitrogen. One major obstacle for their large-scale implementation is the scarcity of cost-effective, durable, and efficient catalysts. A family of two-dimensional transition metal carbides, nitrides, and carbonitrides (MXenes) has recently emerged as promising earth-abundant candidates for large-area catalytic energy storage and conversion due to their unique properties of hydrophilicity, high metallic conductivity, and ease of production by solution processing. To take full advantage of these desirable properties, MXenes have been combined with other materials to form MXene hybrids with significantly enhanced catalytic performances beyond the sum of their individual components. MXene hybridization tunes the electronic structure toward optimal binding of redox active species to improve intrinsic activity while increasing the density and accessibility of active sites. This review outlines recent strategies in the design of MXene hybrids for industrially relevant electrocatalytic, photocatalytic, and photoelectrocatalytic applications such as water splitting, metal-air/sulfur batteries, carbon dioxide reduction, and nitrogen reduction. By clarifying the roles of individual material components in the MXene hybrids, we provide design strategies to synergistically couple MXenes with associated materials for highly efficient and durable catalytic applications. We conclude by highlighting key gaps in the current understanding of MXene hybrids to guide future MXene hybrid designs in catalytic energy storage and conversion applications.

/pdf/rational-design-of-two-dimensional-transition-metal-carbide-475jnshg2v.pdf

Rational Design of Two-Dimensional Transition Metal Carbide/Nitride (MXene) Hybrids and Nanocomposites for Catalytic Energy Storage and Conversion

2D transition metal carbides and/or nitrides (MXenes), by virtue of high electrical conductivity, abundant surface functional groups and excellent dispersion in various solvents, are attracting increasing attention and showing competitive performance in energy storage and conversion applications. However, like other 2D materials, MXene nanosheets incline to stack together via van der Waals interactions, which lead to limited number of active sites, sluggish ionic kinetics, and finally ordinary performance of MXene materials/devices. Constructing 2D MXene nanosheets into 3D architectures has been proven to be an effective strategy to reduce restacking, thus providing larger specific surface area, higher porosity, and shorter ion and mass transport distance over normal 1D and 2D structures. In this review, the commonly used strategies for manufacturing 3D MXene architectures (3D MXenes and 3D MXene‐based composites) are summarized, such as template, assembly, 3D printing, and other methods. Special attention is also given to the structure–property relationships of 3D MXene architectures and their applications in electrochemical energy storage and conversion, including supercapacitors, rechargeable batteries, and electrocatalysis. Finally, the authors propose a brief perspective on future opportunities and challenges for 3D MXene architectures/devices.

/pdf/3d-mxene-architectures-for-efficient-energy-storage-and-4jfj4vbd2z.pdf

3D MXene Architectures for Efficient Energy Storage and Conversion

Lithium–sulfur batteries (Li–S) have become a viable alternative to future energy storage devices. The electrochemical reaction based on lithium and sulfur promises an extraordinary theoretical energy density, which is far higher than current commercialized Li-ion batteries. However, the principal disadvantage impeding the success of Li–S batteries lies in the severe leakage and migration of soluble lithium polysulfide intermediates out of cathodes upon cycling. The loss of active sulfur species incurs significant capacity decay and poor battery lifespans. Considerable efforts have been devoted to developing various sulfur host materials that can effectively anchor lithium polysulfides. Herein, a comprehensive review is presented of recent advances in sulfur host materials. On the basis of the electrochemistry of Li–S batteries, the strategies for anchoring polysulfides are systematically categorized into physical confinement and chemical bonding. The structural merits of various sulfur host materials are highlighted, and the interaction mechanisms with sulfur species are discussed in detail, which provides valuable insights into the rational design and engineering of advanced sulfur host materials facilitating the commercialization of Li–S batteries. Future challenges and promising research prospects for sulfur host materials are proposed at the end of the review.

Host Materials Anchoring Polysulfides in Li–S Batteries Reviewed

In lithium-sulfur batteries, small S2–4 molecules show very different electrochemical responses from the traditional S8 material. Their exact lithiation/delitiation mechanism is not clear and how to select proper electrolytes for the S2–4 cathodes is also ambiguous. Here, S2–4 and S8/S2–4 composites with highly ordered microporous carbon as a confining matrix are fabricated and the electrode mechanism of the S2–4 cathode is investigated by comparing the electrochemical performances of the S2–4 and S2–4/S8 electrodes in various electrolytes combined with theoretical calculation. Experimental results show that the electrolyte and microstructure of carbon matrix play important roles in the electrochemical performance. If the micropores of carbon are small enough to prevent the penetration of the solvent molecules, the lithiation/delithiation for S2–4 occurs as a solid-solid process. The irreversible chemically reactions between the polysulfudes and carbonates, and the dissolution of the polysulfides into the ethers can be effectively avoided due to the steric hindrance. The confined S2–4 show high adaptability to the electrolytes. The sulfur cathode based on this strategy exhibits excellent rate capability and cycling stability.

Insight Into the Electrode Mechanism in Lithium-Sulfur Batteries With Ordered Microporous Carbon Confined Sulfur As Cathode

Research on next-generation battery technologies (beyond Li-ion batteries, or LIBs) has been accelerating over the past few years. A key challenge for these emerging batteries has been the lack of suitable electrode materials, which severely limits their further developments. MXenes, a new class of 2D transition metal carbides, carbonitrides, and nitrides, are proposed as electrode materials for these emerging batteries due to several desirable attributes. These attributes include large and tunable interlayer spaces, excellent hydrophilicity, extraordinary conductivity, compositional diversity, and abundant surface chemistries, making MXenes promising not only as electrode materials but also as other components in the cells of emerging batteries. Herein, an overview and assessment of the utilization of MXenes in rechargeable batteries beyond LIBs, including alkali-ion (e.g., Na+ , K+ ) storage, multivalent-ion (e.g., Mg2+ , Zn2+ , and Al3+ ) storage, and metal batteries are presented. In particular, the synthetic strategies and properties of MXenes that enable MXenes to play various roles as electrodes, metal anode protective layers, sulfur hosts, separator modification layers, and conductive additives in these emerging batteries are discussed. Moreover, a perspective on promising future research directions on MXenes and MXene-based materials, ranging from material design and processing, fundamental understanding of the reaction mechanisms, to device performance optimization strategies is provided.

MXenes for Rechargeable Batteries Beyond the Lithium-Ion

Dissolution of lithium polysulfides (LiPSs), volume expansion, and the insulative nature of elemental sulfur are the major challenges for high-performance lithium sulfur batteries (LSBs). To mitiga...

Self-Assembled 3D MnO2 Nanosheets@Delaminated-Ti3C2 Aerogel as Sulfur Host for Lithium–Sulfur Battery Cathodes

Lithium–sulfur (Li–S) batteries are regarded as potential next-generation energy storage systems due to their high theoretical energy densities. However, the dissolution of lithium polysulfides (LiPSs) upon cycling can result in severe capacity degradation. Achieving high rate capabilities with good cycling stability remains a huge obstacle for the practical implementation of Li–S batteries. Here we developed a novel, multifunctional, hierarchical structure by self-assembling core–shell MnO2 nanorods @ hollow porous carbon with 2D Ti3C2Tx nanosheets, labelled as MCT, as an efficient polysulfide mediator for Li–S cathodes. The integration of the polar MnO2 core and hollow porous carbon shell captures LiPSs two ways: physical confinement and chemisorption. The conductive Ti3C2Tx nanosheets construct a continuous and conductive network, which not only promotes charge transfer and ion diffusion but also boosts LiPS adsorption and conversion. Based on these merits, the MCT/S cathode delivers good rate capability (688 mA h g−1 at 2.0C) and outstanding long-term cyclability (0.044% capacity decay per cycle over 600 cycles at 2.0C).

Ti3C2Tx nanosheet wrapped core-shell MnO2 nanorods @ hollow porous carbon as a multifunctional polysulfide mediator for improved Li-S batteries.

Synthesis of CdSe Nanowires and CuInSe2 Nanosheets for Hydrogen Evolution

Self-assembled sandwich hollow porous carbon sphere @ MXene composites as superior LiS battery cathode hosts

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Self-Assembled 3D MnO2 Nanosheets@Delaminated-Ti3C2 Aerogel as Sulfur Host for Lithium–Sulfur Battery Cathodes

Ti3C2Tx nanosheet wrapped core-shell MnO2 nanorods @ hollow porous carbon as a multifunctional polysulfide mediator for improved Li-S batteries.

Synthesis of CdSe Nanowires and CuInSe2 Nanosheets for Hydrogen Evolution

Self-assembled sandwich hollow porous carbon sphere @ MXene composites as superior LiS battery cathode hosts