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

Recent Progress in MXene-Based Materials: Potential High-Performance Electrocatalysts

Most recently, two-dimensional (2D) transition-metal carbides (MXenes) have been demonstrated to be promising electrocatalysts owing to their unique chemical and electronic properties, e.g., metallic conductivity, high hydrophilicity, and tunable surface terminations. Herein, representative progress achieved in MXenes as hydrogen evolution reaction electrocatalysts is reviewed both experimentally and theoretically. Briefly, termination modification and heteroatom incorporation are applied to optimize the chemical and electronic configurations of active sites for intrinsically enhanced catalytic kinetics while various nanostructures and hybridizations are fabricated to increase the density and accessibility of active sites. Then, the achievements of MXene-based catalysts in other electrocatalysis processes are also summarized, including the oxygen evolution/reduction reaction, carbon dioxide reduction reaction and nitrogen reduction reaction. Finally, current challenges and future research directions for MXene-based electrocatalysis are discussed.

Recent advances in structural engineering of MXene electrocatalysts

Two-dimensional materials have gained immense attention for technological applications owing to their characteristic properties. MXene is one of the fast-growing family of 2D materials that exhibits remarkable physiochemical properties that cater numerous applications in the field of energy and storage. This review comprises the significant advancement in the field of 2D MXene and discusses the evolution of the design, synthetic strategies, and stability. In addition to illuminating the state-of-the-art applications, we discuss the challenges and limitations that preclude the scientific fraternity from realizing functional MXene with controlled structures and properties for renewable clean energy conversion and storage applications.

/pdf/prospects-challenges-and-stability-of-2d-mxenes-for-clean-24upw8jgcy.pdf

Prospects challenges and stability of 2D MXenes for clean energy conversion and storage applications

The development of highly efficient and durable earth-abundant hydrogen evolution reaction (HER) catalysts is crucial for the extensive implementation of the hydrogen economy. Members of the 2D MXenes family, particularly Mo2CTx, have recently been identified as promising HER catalysts. However, their inherent oxidative instability in air and aqueous electrolyte solutions is hindering their widespread use. Herein, we present a simple and scalable method to circumvent adventitious oxidation in Mo2CTx MXenes via in situ sulfidation to form a Mo2CTx/2H-MoS2 nanohybrid. The intimate epitaxial coupling at the Mo2CTx/2H-MoS2 nanohybrid interface afforded superior HER activities, requiring only 119 or 182 mV overpotential to yield -10 or -100 mA cm-2geom current densities, respectively. Density functional theory calculations reveal strongest interfacial adhesion was found within the nanohybrid structure as compared to the physisorbed nanohybrid, and the possibility to tune the HER overpotential through manipulating the extent of MXene sulfidation. Critically, the presence of 2H-MoS2 suppresses further oxidation of the MXene layer, enabling the nanohybrid to sustain industrially relevant current densities of over -450 mA cm-2geom with exceptional durability. Less than 30 mV overpotential degradation was observed after 10 continuous days of electrolysis at a fixed -10 mA cm-2geom current density or 100,000 successive cyclic voltammetry cycles. The exceptional HER durability of the Mo2CTx/2H-MoS2 nanohybrid presents a major step forward to realize practical implementation of MXenes as noble metal free catalysts for broad-based applications in water splitting and energy conversion.

2H-MoS2 on Mo2CTx MXene Nanohybrid for Efficient and Durable Electrocatalytic Hydrogen Evolution.

Two-dimensional molybdenum carbides belong to a novel family of 2D transition metal carbides/nitrides called MXenes, which have a wide range of electrochemical applications. However, the synergistic catalysis of transition metal carbides and disulfides has not been studied in depth. A strategy was proposed to prepare a 2D organ-like Mo2C MXene matrix derived from Mo2Ga2C crystals, coupled with MoS2 nanoflowers to explore the hydrogen evolution reaction (HER) of molybdenum carbides and disulfides. Compared with Mo2CTx (where Tx means F, O, and OH surface terminations) Mxene catalysts, MoS2@Mo2CTx nanohybrids showed significantly enhanced HER activity, with a low overpotential of 176 mV in alkaline media at a current density of 10 mA cm−2 and a very small overpotential of 26 Ω. Density functional theory calculations indicated that the reduction of the hydrogen adsorption energy of the MoS2@Mo2CTx nanohybrids could be attributed to fast electron transport ensured by Mo2CTx with intrinsic conductivity and a large number of hydrogen adsorption sites provided by MoS2 nanoflowers. The synthetic method is promising to tailor the specific properties by preparing organ-like molybdenum carbides coupled with MoS2 nanoflowers.

2D organ-like molybdenum carbide (MXene) coupled with MoS2 nanoflowers enhances the catalytic activity in the hydrogen evolution reaction

Metal-organic frameworks-derived CoP anchored on MXene toward an efficient bifunctional electrode with enhanced lithium storage

Herein, in order to overcome the poor conductivity and pH limitation of MoS2 in electrocatalytic applications, a MoS2/Nb2CTx heterostructure was synthesized for the first time via an easy hydrothermal method and first-principles investigation was further carried out. The MoS2/Nb2CTx contact shows a metallic property, which guarantees excellent conductivity. Meanwhile, the low p-type Schottky barrier contact on the interface leads to efficient charge transfer from Nb2CTx to MoS2 and further improves its ability to adsorb hydrogen. As a result, the composite showed a low overpotential of 127 mV at 10 mA cm−2, Tafel slope of 56.3 mV dec−1 in acidic solution and an overpotential of 138.8 mV at 10 mA cm−2, and Tafel slope of 93.4 mV dec−1 in alkaline solution. In both solutions, it showed outstanding stability after 3000 cycles. Both experimental and theoretical investigation in our work revealed the potential of this composite for hydrogen evolution reaction in both acidic and alkaline media and provided an effective route to design high-performance MoS2-based catalysts.

Experimental and theoretical investigation on MoS2/MXene heterostructure as an efficient electrocatalyst for hydrogen evolution in both acidic and alkaline media

In this work, we present an interfacial superassembly by engineering MoSe2 nanoflowers coupled with ribbon-like Ti2N MXene frameworks (MoSe2@Ti2N MXene). The MoSe2@Ti2N MXene hybrids have excellent electrochemical performance and are used as anode materials for lithium-ion batteries (LIBs). Etching the Ti2AlN precursor under different conditions results in two kinds of novel materials with different morphologies: sliced etched-Ti2N and ribbon-like Ti2N MXene. Electrochemical analysis indicates that the ribbon-like Ti2N MXene frameworks not only help to avoid side reactions on carbides in LIBs, but also contribute to the outstanding rate capacity and superior specific capacity, thus achieving ultra-stable long-life cycling performance. The distinctive flower-like MoSe2 can be assembled onto the ribbon-like Ti2N MXene substrate by the interfacial superassembly. The MoSe2@Ti2N MXene electrode reveals a reversible specific capacity of 826 mAh g−1 at a current density of 0.1 A g−1 after 200 cycles. It maintains a capacity of 489 mAh g−1 after 2000 cycles at 1.0 A g−1 indicating satisfactory cycling stability. The new-type interfacial superassembly can provide a novel synthesis strategy for anode electrodes to improve the performance of LIBs.

Interfacial superassembly of MoSe2@Ti2N MXene hybrids enabling promising lithium-ion storage

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2D organ-like molybdenum carbide (MXene) coupled with MoS2 nanoflowers enhances the catalytic activity in the hydrogen evolution reaction

Metal-organic frameworks-derived CoP anchored on MXene toward an efficient bifunctional electrode with enhanced lithium storage

Experimental and theoretical investigation on MoS2/MXene heterostructure as an efficient electrocatalyst for hydrogen evolution in both acidic and alkaline media

Interfacial superassembly of MoSe2@Ti2N MXene hybrids enabling promising lithium-ion storage