MXenes, the largest and most diverse group of emerging two-dimensional materials, have potentials across multiple applications. The increasing attention is driven by the fascinating tunable surface properties, and synergetic chemistry facilitated by the presence of multiple chemical bonds dominated by covalent and metallic bonds between transition metals (M) and non-metals, X (such as carbon, nitrogen, or both). Although the various available synthesis approaches offer opportunities for tuning MXenes for specific applications, their inherent environmental and toxicity risks as well as poor scale-up potential are currently hampering research and commercialization progress. Therefore, ongoing efforts are focused on developing less hazardous, scalable methodologies to limit the barriers. This review comprehensively surveys the literature from the seminal MXene paper to the present, offering insights into the factors, latest advancements, limitations, trends, and existing gaps in MXene synthesis, properties, and applications in the areas of environment and energy storage. Special emphasis is placed on the need to address environmental concerns associated with fluoride-based synthesis while an overview of safer, non-fluoride alternatives is provided. Furthermore, the most recent breakthroughs in scalable top-down dry selective etching (DSE), bottom-up solid-state direct synthesis, and structural editing protocol using chemical scissors are presented. In particular, this review critically examines the current state of knowledge and identifies key research progresses and areas that deserve intensive attention to facilitate safe and industrial-scale synthesis and application of MXenes for catalysis, environmental remediation, and energy storage. Addressing the identified gaps will accelerate the transformation of MXenes and their composites into the components of our everyday appliances. 

MXenes: Synthesis, properties, and applications for sustainable energy and environment

The direct pyrolysis of metal-zeolite imidazolate frameworks (M-ZIFs) has been widely recognized as the predominant approach for synthesizing atomically dispersed metal-nitrogen-carbon single-atom catalysts (M/NC-SACs), which have exhibited exceptional activity and selectivity in the semihydrogenation of acetylene. However, due to weak adsorption of reactants on the single site and restricted molecular diffusion, the semihydrogenation of large organic molecules (e.g., phenylacetylene) was greatly limited for M/NC-SACs. In this work, a dual single-atom catalyst (h-Pd-Mn/NC) with hollow mesopores was designed and prepared using a general host-guest strategy. Taking the semihydrogenation of phenylacetylene as an example, this catalyst exhibited ultrahigh activity and selectivity, which achieved a turnover frequency of 218 molC═CmolPd-1 min-1, 16-fold higher than that of the commercial Lindlar catalyst. The catalyst maintained high activity and selectivity even after 5 cycles of usage. The superior activity of h-Pd-Mn/NC was attributed to the 4.0 nm mesopore interface of the catalyst, which enhanced the diffusion of macromolecular reactants and products. Particularly, the introduction of atomically dispersed Mn with weak electronegativity in h-Pd-Mn/NC could drive the electron transfer from Mn to adjacent Pd sites and regulate the electronic structure of Pd sites. Meanwhile, the strong electronic coupling in Pd-Mn pairs enhanced the d-electron domination near the Fermi level and promoted the adsorption of phenylacetylene and H2 on Pd active sites, thereby reducing the energy barrier for the semihydrogenation of phenylacetylene.

Pd-Mn/NC Dual Single-Atomic Sites with Hollow Mesopores for the Highly Efficient Semihydrogenation of Phenylacetylene.

Efficient catalysts with minimal content of catalytically active noble metals are essential for the transition to the clean hydrogen economy. Catalyst supports that can immobilize and stabilize catalytic nanoparticles and facilitate the supply of electrons and reactants to the catalysts are needed. Being hydrophilic and more conductive compared with carbons, MXenes have shown promise as catalyst supports. However, the controlled assembly of their 2D sheets creates a challenge. This study established a lattice engineering approach to regulate the assembly of exfoliated Ti3C2Tx MXene nanosheets with guest cations of various sizes. The enlargement of guest cations led to a decreased interlayer interaction of MXene lamellae and increased surface accessibility, allowing intercalation of Pd nanoparticles. Stabilization of Pd nanoparticles between interlayer-expanded MXene nanosheets improved their electrocatalytic activity. The Pd-immobilized K+-intercalated MXene nanosheets (PdKMX) demonstrated exceptional electrocatalytic performance for the hydrogen evolution reaction with the lowest overpotential of 72 mV (@10 mA cm-2) and the highest turnover frequency of 1.122 s-1 (@ an overpotential of 100 mV), which were superior to those of the state-of-the-art Pd nanoparticle-based electrocatalysts. Weakening of the interlayer interaction during self-assembly with K+ ions led to fewer layers in lamellae and expansion of the MXene in the c direction during Pd anchoring, providing numerous surface-active sites and promoting mass transport. In situ spectroscopic analysis suggests that the effective interfacial electron injection from the Pd nanoparticles strongly immobilized on interlayer-expanded PdKMX may be responsible for the improved electrocatalytic performance.

Enhancing Hydrogen Evolution Reaction Activity of Palladium Catalyst by Immobilization on MXene Nanosheets.

MXenes are a class of 2D materials that include layered transition metal carbides, nitrides, and carbonitrides. Since their inception in 2011, they have garnered significant attention due to their diverse compositions, unique structures, and extraordinary properties, such as high specific surface areas and excellent electrical conductivity. This versatility has opened up immense potential in various fields, catalyzing a surge in MXene research and leading to note worthy advancements. This review offers an in-depth overview of the evolution of MXenes over the past 5 years, with an emphasis on synthetic strategies, structure-property relationships, and technological prospects. A classification scheme for MXene structures based on entropy is presented and an updated summary of the elemental constituents of the MXene family is provided, as documented in recent literature. Delving into the microscopic structure and synthesis routes, the intricate structure-property relationships are explored at the nano/micro level that dictate the macroscopic applications of MXenes. Through an extensive review of the latest representative works, the utilization of MXenes in energy, environmental, electronic, and biomedical fields is showcased, offering a glimpse into the current technological bottlenecks, such asstability, scalability, and device integration. Moreover, potential pathways for advancing MXenes toward next-generation technologies are highlighted.

Functional MXenes: Progress and Perspectives on Synthetic Strategies and Structure-Property Interplay for Next-Generation Technologies.

Electrocatalytic alkynol semi‐hydrogenation for the high‐value chemicals alkenol with mild conditions and carbon‐free emission is a potentially green and sustainable alternative to conventional thermocatalytic routes, which generally involves the design of electrocatalysts with high activity and high selectivity. Here, the rare‐earth single‐atom (Ln = La, Nd, Pr) coordinated Pd metallene (Ln1Pdene) is reported for electrocatalytic 2‐methyl‐3‐butyn‐2‐ol (MBY) semi‐hydrogenation reaction (MBY ESHR) to synthesis of 2‐methyl‐3‐buten‐2‐ol (MBE). Typically, in alkaline medium containing 0.1 m MBY, MBY conversion and MBE selectivity of La1Pdene are as high as ≈97% and ≈95%, respectively, with excellent electrocatalytic stability. Meanwhile, in situ infrared spectra reveal the conversion of MBY to MBE during the dynamic electrocatalytic process. Theoretical calculations reveal that the interaction between La single‐atom and Pd host triggers an unconventional transformation of the intermediate MBE* adsorption configuration during electrocatalytic hydrogenation, achieving the optimal desorption energy between La1Pd and target product and optimizing the reaction energy barriers to inhibit the over‐hydrogenation of MBE. Moreover, La single‐atom as the adsorption active site of the hydrogen supplier H2O effectively reduces the competition adsorption between the reactants MBY and H2O, rendering La single‐atom and Pd host as the synergistic co‐catalytic active sites to promote the electrocatalytic MBY semi‐hydrogenation reaction.

High‐Density Rare‐Earth Single‐Atom‐Triggered Unconventional Transition of Adsorption Configuration on La1Pd Monatomic Alloy Metallene for Sustainable Electrocatalytic Alkynol Semi‐Hydrogenation

2D metallene nanomaterials have spurred considerable attention in heterogeneous catalysis by virtue of sufficient unsaturated metal atoms, high specific surface area and surface strain. Nevertheless, the strong metallic bonding in nanoparticles aggravates the difficulty in the controllable regulation of the geometry of metallenes. Here we propose an efficient galvanic replacement strategy to construct Pd metallenes loaded on Nb2C MXenes at room temperature, which is triggered by strong metal-support interaction based on MD simulations. The Pd metallenes feature a chair structure of six-membered ring with the coordination number of Pd as low as 3. Coverage-dependent kinetic analysis based on first-principles calculations reveals that the tripodal Pd metallenes promote the diffusion of alkene and inhibit its overhydrogenation. As a consequence, Pd/Nb2C delivers an outstanding turnover frequency of 10372 h-1 and a high selectivity of 96% at 25 oC in the semihydrogenation of alkynes without compromising the stability. This strategy is general and scalable considering the plentiful members of the MXene family, which can set a foundation for the design of novel supported-metallene catalysts for demanding transformations. 

/pdf/tripodal-pd-metallenes-mediated-by-nb2c-mxenes-for-boosting-kd60omkh.pdf

Tripodal Pd metallenes mediated by Nb2C MXenes for boosting alkynes semihydrogenation

Achieving precise control of reaction selectivity at high conversion levels is crucial for semi-hydrogenation of alkyne. In this study, three kinds of Pd/Nb2C catalysts (NaBH4-Pd/Nb2C, Pyrolysis-Pd/Nb2C, and H2-Pd/Nb2C) with different degree of SMSI were elaborately designed by tailoring the reduction mode of Pd on Nb2C. H2-Pd/Nb2C with the strongest SMSI displayed an exceptional TOF (7263 h−1) of phenylacetylene and high selectivity (93.5 %) towards styrene, achieving a fine equilibrium between high activity and selectivity. The outstanding performance of H2-Pd/Nb2C can be ascribed to the facilitated electron transfer from Nb to Pd, thus forming an electron-rich Pd and specific Pd-Nb2C interface. Moreover, the promotion effect in catalytic activity caused by the expansion of Nb2C layer spacing is linearly related to the molecular diameter of the reactants. With the increase of interlayer spacing, the more significant the enhancement in catalytic activity of Pd/Nb2C catalyst for the substrates with larger diameter. 

Adjustable metal-support interaction and interlayer spacing of Pd/MXenes boosting alkyne semi-hydrogenation via enhanced reaction and diffusion

Cooperative Effect of Pd2+ and Pd0 in Selective Hydrogenation of Nitrile Rubber

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Tripodal Pd metallenes mediated by Nb2C MXenes for boosting alkynes semihydrogenation

Adjustable metal-support interaction and interlayer spacing of Pd/MXenes boosting alkyne semi-hydrogenation via enhanced reaction and diffusion

Cooperative Effect of Pd2+ and Pd0 in Selective Hydrogenation of Nitrile Rubber