Efficient Reaction Research Articles

Two-Dimensional Perovskites for Photocatalytic CO2 Reduction.

The photocatalytic conversion of Carbon dioxide (CO2) into valuable chemicals is one of the most promising approaches for addressing the CO2 emission problem. However, several issues still need to be resolved to increase the efficiency of photocatalytic reaction. Perovskites possess superior light absorption capacity, tunable band gap, high defect tolerance, and diverse dimensionality. Among them, two-dimensional (2D) perovskites are more stable under photocatalytic conditions and have an exciting excitonic characteristics compared to three-dimensional (3D) perovskites. 2D perovskites have unique physical and chemical properties, such as, high stability, polaron formation, quantum well structures, and high exciton binding energies, which remain underexplored for photocatalytic CO2 reduction (pCO2RR). Tuning of these properties is easier in 2D perovskites than 3D perovskites by varying the layer thickness and spacer cations. Therefore, 2D perovskites photocatalysts are emerging as promising materials for reducing CO2 into valuable products. This review discusses the classification and synthesis methods for 2D perovskites, the unique properties that make it favorable for photocatalysis, and recent advances in applying 2D perovskites for pCO2RR by monitoring the operational methodology. It also emphasizes potential for future developments in photocatalysis using 2D perovskites.

Microbubble-enhanced plasma water-based nitrogen fixation: generation mechanisms, regulation strategies, and application prospects

Abstract This study introduces the solar-powered microbubble-enhanced plasma water-based nitrogen fixation (MEPWBNF) technology, a novel and environmentally friendly approach to nitrogen fixation that offers high efficiency. By employing Venturi tubes to produce a continuous flow of microbubbles, this technology significantly enhances the interaction between gaseous plasma nitrogen compounds and water, leading to improved solubility and reaction efficiency of nitrogen compounds in water. Comparative analyses reveal that MEPWBNF achieves a 33.7% reduction in energy consumption and a 52.8% increase in yield compared to traditional PWBNF methods without microbubble-enhanced method. Moreover, the resulting plasma-activated tap water can be directly utilized as a nutrient solution in hydroponic systems, effectively boosting lettuce growth. The adoption of MEPWBNF technology presents a promising strategy for reducing agricultural dependence on chemical fertilizers and advancing sustainable farming practices.

Revealing the origin of activity and selectivity in nitrate to ammonia conversion on single transition metal atom catalysts supported by a Ti2NO2 monolayer.

In recent years, the issue of nitrate (NO3-) contamination has become an increasingly severe problem for human life. Electrocatalytic nitrate reduction to ammonia (NH3) is one of the promising strategies to eliminate nitrate contamination. However, the reduction of NO3- to NH3 is a multi-electron process and is susceptible to interference from by-products and competing hydrogen evolution reactions (HER). Introducing a single transition metal (TM) atom onto MXene-based surfaces can alter MXenes' electronic configuration, enhancing their catalytic performance and the Faraday efficiency of the nitrate reduction reaction (NO3RR). In this work, we investigated the initial activation mechanisms of nitrate on various TM-modified Ti2NO2 (TM@Ti2NO2) catalysts and their NO3RR performance using first-principles calculations, aiming to select effective NO3RR electrocatalysts. The results indicated that both V@Ti2NO2 and Cr@Ti2NO2 were viable catalysts for NO3RR, showing particular promise for the efficient conversion of NO3- to NH3 at the most favorable limiting potentials of -0.41 V and -0.52 V, respectively. Further electronic structure analysis (density of states, COHP, and the descriptor ψ) confirmed that the single TM atom supported the boost in product selectivity and efficiency of NH3 by acting as an electron "bridge" to strengthen the interaction between NO3- and MXenes. AIMD simulations indicated that V@Ti2NO2 and Cr@Ti2NO2 maintained dynamical stability at the reaction temperature. These findings lay the foundation for a deeper understanding of the initial activation mechanisms and provide fresh theoretical insights into the design of MXene-based electrocatalysts with high NO3RR performance.

Chirality Assisted Triplet Electron Pairing.

Redox processes that involve pairs of electrons are common in nature. Some of these reactions involve oxygen molecules. The understanding of the efficiency of the oxygen reduction reaction (ORR), for example, is a challenge since the reaction is spin forbidden and requires the transfer of two pairs of electrons. Past experimental and theoretical studies demonstrated that by controlling the spin of the transferred electrons, it is possible to overcome the barrier resulting from the spin mismatch between the reactants and the products. In other works, it was suggested that the reaction is enhanced if the two electrons in each pair have phase relation, namely, they possess the property of a triplet state. Since in nature electrons are transferred through chiral systems, we probed if chirality affects the formation of paired electrons with the same spin, namely, a triplet like state. The model calculations demonstrate that chirality enhances the probability of the formation of electron pairing in the triplet states, even at room temperature. This enhancement originates from breaking the spin degeneracy, enabled by chirality and interaction of the spins with vibrations.

Integrating Two Photochromics into One Three-Dimensional Covalent Organic Framework for Synergistically Enhancing Multiple Photocatalytic Oxidations.

While photocatalytic oxidations are a category of important reactions in wide chemical synthesis, the fabrication of effective photocatalysts for broad oxidation reactions is still of a great challenge. Herein, by rationally integrating two photochromics, porphyrin and triphenylamine, a three-dimensional photoactive covalent organic framework (COF) is successfully constructed for photocatalytic oxidations. Characterization studies not only show the formation of a crystalline and three-dimensional porous framework, but also reveal its effective photochemical semiconductor properties derived from the porphyrin and triphenylamine moieties. Electron paramagnetic resonance measurements indicate that the COF is an effective photocatalyst for the generation of both singlet oxygen (1O2) and superoxide radical anions (·O2-). Synergistically enhanced efficiency in all photocatalytic reactions of photocatalytic aerobic oxidation of alkylbenzenes and silanes as well as thioanisoles, and cross-dehydrogenative coupling reaction of N-phenyltetrahydroisoquinoline and indole is confirmed by both experimental and theoretical studies, demonstrating its promising potential for broad photocatalytic oxidation reactions.

Integrating Two Photochromics into One Three‐Dimensional Covalent Organic Framework for Synergistically Enhancing Multiple Photocatalytic Oxidations

While photocatalytic oxidations are a category of important reactions in wide chemical synthesis, the fabrication of effective photocatalysts for broad oxidation reactions is still of a great challenge. Herein, by rationally integrating two photochromics, porphyrin and triphenylamine, a three‐dimensional photoactive covalent organic framework (COF) is successfully constructed for photocatalytic oxidations. Characterization studies not only show the formation of a crystalline and three‐dimensional porous framework, but also reveal its effective photochemical semiconductor properties derived from the porphyrin and triphenylamine moieties. Electron paramagnetic resonance measurements indicate that the COF is an effective photocatalyst for the generation of both singlet oxygen (1O2) and superoxide radical anions (·O2−). Synergistically enhanced efficiency in all photocatalytic reactions of photocatalytic aerobic oxidation of alkylbenzenes and silanes as well as thioanisoles, and cross‐dehydrogenative coupling reaction of N‐phenyltetrahydroisoquinoline and indole is confirmed by both experimental and theoretical studies, demonstrating its promising potential for broad photocatalytic oxidation reactions.

Robust Coupling Between Piezoelectric Field and Interfacial Polarization in Layered Bismuth-Based Heterostructure for High-performance Piezocatalytic Water Splitting.

The creation of heterostructures with inherent interface polarization has been proven effective in enhancing piezocatalytic activity; however, developing efficient heterostructure piezocatalysts remains challenging, and the underlying mechanisms are not well understood. In this work, a stable Bi2WO6/BiOBr heterostructure with strong chemical binding is successfully constructed by exchanging double Br- with WO4 2- in hydrothermal reaction. The heterostructure demonstrates exceptional piezocatalytic hydrogen evolution reaction (HER) efficiencies of 0.75mmol g⁻¹ h⁻¹ in water and 2.28mmol g⁻¹ h⁻¹ in methanol solution, respectively, outperforming the majority of recently reported bismuth-based piezocatalysts. During piezocatalytic operations, a robust coupling between the stress-induced piezoelectric field and the inherent interfacial polarization is pivotal. This coupling results in a large intrinsic dipole moment, excellent piezoelectricity, and improved carrier separation and transfer. Additionally, the polar surface of heterostructure facilitates decreased Gibbs free energy, increased surface potential, and reduced charge transfer resistance, all of which contribute to the high-activity surface piezocatalytic reaction. This study introduces a simple and universal method for in situ construction of layered bismuth-based heterostructures with high piezocatalytic performance and offers valuable insights into the role of polarization coupling in piezocatalysis.

Engineering DNA Nanodevices with Multi-site Recognition and Multi-signal Output for Accurate Intracellular LncRNA Imaging.

Dynamic DNA nanodevices, known for their high programmability and controllability, are pivotal in intracellular biomarker imaging. However, these nanodevices often suffer from inadequate detection sensitivity and specificity due to limited cellular loading capacity and low signal feedback. Herein, we engineered an integrated multi-site recognition and multi-signal output of four-leaf clover dynamic DNA nanodevice (MEMORY) that enables sensitive and accurate intracellular long noncoding RNA (lncRNA) imaging. MEMORY features one fluorophore (FAM)-modified cross-shaped structure as spatial-confinement scaffolds loaded with four identical quenchers (BHQ1)-modified recognition probes (RPs), ensuring a low background signal initially. In the presence of target lncRNA, the multiple recognition sites of MEMORY facilitate hybridization with the target to selectively release the RPs, exposing the toehold region and outputting the green fluorescence (FAM) signal. Furthermore, the exposed toehold region can trigger efficient and rapid hybridization chain reaction (HCR) amplification, outputting the red fluorescence (Cy5) signal. MEMORY's multiple recognition sites increase the likelihood of target collisions, enhancing reaction efficiency, while its multi-signal output provides sequential feedback through FAM and Cy5, boosting overall signal intensity. With the lncRNA metastasis-related lung adenocarcinoma transcript 1 (MALAT1) as a detection model, MEMORY offers a linear detection range from 1 pM to 100 nM, with a limit of detection of 0.29 pM. We demonstrated that MEMORY can differentiate between normal and tumor cells based on intracellular MALAT1 imaging. This integrated DNA nanodevice will offer valuable tools for sensitive and accurate imaging of intracellular biomarkers.

Recent Developments in SERS Microfluidic Chips: From Fundamentals to Biosensing Applications.

This paper reviews the latest research progress of surface-enhanced Raman spectroscopy (SERS) microfluidic chips in the field of biosensing. Due to its single-molecule sensitivity, selectivity, minimal or no preprocessing, and immediacy, SERS is considered a promising biosensing technology. However, the nondirectional interactions between biological samples and the substrate, as well as fluctuations in the sample environment temperature during signal acquisition, can affect the stability and reproducibility of SERS signals. Integrating SERS spectroscopy with microfluidic chips not only leverages the continuous sample flow, high reaction efficiency, high throughput, and multifunctionality of microfluidic chips to address challenges in biosensing applications but also expands the scope of microfluidic technology by providing a novel on-chip optical detection method. The combination of SERS and microfluidic chips not only enables the complementary advantages of both technologies but also offers a highly promising "combined technology" for the field of biosensing. This paper starts by introducing the enhancement mechanisms of SERS and presents both labeled and label-free SERS strategies. Based on the differences in substrate properties, we broadly categorize SERS microfluidic chips into colloidal nanoparticle-based SERS microfluidic chips and fixed substrate-based SERS microfluidic chips. Finally, we review the latest research progress on SERS microfluidic chips for biosensing biological targets such as nucleic acids, proteins, small biomolecules, and live cells. In the conclusion and outlook section, we summarize the challenges faced by SERS microfluidic chips in biosensing and propose feasible solutions. To better leverage the role of SERS microfluidic chips in biosensing, we also present an outlook on the future development of this combined technology.

Coalescence of carbon nanotubes while preserving the chiral angles.

Atomically precise coalescence of graphitic nanocarbon molecules is one of the most challenging reactions in sp2 carbon chemistry. Here, we demonstrate that two carbon nanotubes with the same chiral indices (n, m) are efficiently coalesced into a single (2n, 2 m) nanotube with preserved chiral angles via heat treatment at less than 1000 °C. The (2n, 2 m) nanotubes constitute up to ≈ 20%-40% of the final sample in the most efficient case. Additional optical absorption peaks of the (2n, 2 m) nanotubes emerge, indicating that the reaction occurs over the entire sample. The reaction efficiency strongly depends on the chiral angle, implying that C-C bond cleavage and recombination occurs sequentially. Furthermore, the reaction occurs efficiently even at 600 °C in an atmosphere containing trace amounts of oxygen. These findings offer routes for the structure-selective synthesis of large-diameter nanotubes and modification of the properties of nanotube assemblies via postprocessing.

Molecular Engineering Spatially Separated Redox Centers Enable Efficient Piezo-Photocatalytic H2O2 Production.

Piezo-photocatalytic production of hydrogen peroxide (H2O2) from water and air is promising but still challenging as insufficient reaction active sites and low reaction efficiency. We have ingeniously applied molecular engineering methods to design an anthraquinone molecularly grafted metal-organic framework piezo-photocatalyst (denoted as UiO-66-AQ) for H2O2 generation from water and air. The catalyst achieves a peak H2O2 yield of 7872.4 μM g-1 h-1, primarily owing to the presence of spatially separated redox sites that enable simultaneously two-step single-electron water oxidation and two-electron oxygen reduction reactions. Notably, experimental and computational simulations confirm rapid carrier separation under the ligand-to-chain charge transfer mode. Electrons transfer to the AQ part and rapidly form internal peroxides for spontaneous oxygen reduction reaction while holes direct to the UiO-66 ligand for the water oxidation reaction. Additionally, a continuous flow tubular reactor with catalytic membranes made of UiO-66-AQ affords 96% removal of organic dyes through the self-Fenton process under visible light and vibrating water flow, confirming the significant potential of the catalyst for practical applications. This work deepens the understanding of directional carrier migration at piezo-photocatalytic spatial separation sites, opening new pathways for environmentally friendly and efficient H2O2 synthesis.

Molecular Engineering Spatially Separated Redox Centers Enable Efficient Piezo‐Photocatalytic H2O2 Production

Piezo‐photocatalytic production of hydrogen peroxide (H2O2) from water and air is promising but still challenging as insufficient reaction active sites and low reaction efficiency. We have ingeniously applied molecular engineering methods to design an anthraquinone molecularly grafted metal‐organic framework piezo‐photocatalyst (denoted as UiO‐66‐AQ) for H2O2 generation from water and air. The catalyst achieves a peak H2O2 yield of 7872.4 μM g‐1 h‐1, primarily owing to the presence of spatially separated redox sites that enable simultaneously two‐step single‐electron water oxidation and two‐electron oxygen reduction reactions. Notably, experimental and computational simulations confirm rapid carrier separation under the ligand‐to‐chain charge transfer mode. Electrons transfer to the AQ part and rapidly form internal peroxides for spontaneous oxygen reduction reaction while holes direct to the UiO‐66 ligand for the water oxidation reaction. Additionally, a continuous flow tubular reactor with catalytic membranes made of UiO‐66‐AQ affords 96% removal of organic dyes through the self‐Fenton process under visible light and vibrating water flow, confirming the significant potential of the catalyst for practical applications. This work deepens the understanding of directional carrier migration at piezo‐photocatalytic spatial separation sites, opening new pathways for environmentally friendly and efficient H2O2 synthesis.

Improving the Methane Oxidation by Self‐Adaptive Optimization of Liquid‐Metal Catalysts

Methane, a major greenhouse gas and abundant carbon resource, presents significant challenges in catalysis due to its high symmetry and thermodynamic stability, which tend to cause over‐oxidation to CO2. Traditional catalysts require high temperatures and pressures to facilitate CH4 conversion, constrained by their rigid structures which lack the flexibility needed for optimizing complex reaction steps. This study introduces a novel Cu single atoms‐embedded liquid metal catalyst (Cu‐LMC) based on gallium alloys, characterized by dynamic, self‐adaptive structures that provide enhanced catalytic performance and selectivity. Our findings reveal that Cu‐LMC achieves a high methane conversion to methanol yield (5.9 mol·gCu‐1·h‐1) with a selectivity of 82%. The results show that mild surface oxidation significantly boosts the catalytic performance of Cu‐LMC by increasing active copper sites through the formation of a Cu‐O‐Ga configuration while preserving the catalyst's structural flexibility. In‐situ XPS and XAFS analyses, along with AIMD simulations, demonstrate that the Cu‐LMC enables self‐adaptive structural adjustments that lower methanol desorption energy and increase the energy barrier for by‐product formation, optimizing the overall methane conversion process. The results underscore the importance of designing catalysts with dynamic and adaptable structures to overcome traditional limitations and improve efficiency in catalytic reactions.

Improving the Methane Oxidation by Self-Adaptive Optimization of Liquid-Metal Catalysts.

Methane, a major greenhouse gas and abundant carbon resource, presents significant challenges in catalysis due to its high symmetry and thermodynamic stability, which tend to cause over-oxidation to CO2. Traditional catalysts require high temperatures and pressures to facilitate CH4 conversion, constrained by their rigid structures which lack the flexibility needed for optimizing complex reaction steps. This study introduces a novel Cu single atoms-embedded liquid metal catalyst (Cu-LMC) based on gallium alloys, characterized by dynamic, self-adaptive structures that provide enhanced catalytic performance and selectivity. Our findings reveal that Cu-LMC achieves a high methane conversion to methanol yield (5.9 mol·gCu-1·h-1) with a selectivity of 82%. The results show that mild surface oxidation significantly boosts the catalytic performance of Cu-LMC by increasing active copper sites through the formation of a Cu-O-Ga configuration while preserving the catalyst's structural flexibility. In-situ XPSand XAFSanalyses, along with AIMD simulations, demonstrate that the Cu-LMC enables self-adaptive structural adjustments that lower methanol desorption energy and increase the energy barrier for by-product formation, optimizing the overall methane conversion process. The results underscore the importance of designing catalysts with dynamic and adaptable structures to overcome traditional limitations and improve efficiency in catalytic reactions.

Bioinspired Nanochitin-Based Porous Constructs for Light-Driven Whole-Cell Biotransformations.

Solid-state photosynthetic cell factories (SSPCFs) are a new production concept that leverages the innate photosynthetic abilities of microbes to drive the production of valuable chemicals. It addresses practical challenges such as high energy and water demand and improper light distribution associated with suspension-based culturing; however, these systems often face significant challenges related to mass transfer. The approach focuses on overcoming these limitations by carefully engineering the microstructure of the immobilization matrix through freeze-induced assembly of nanochitin building blocks. The use of nanochitins with optimized size distribution enabled the formation of macropores with lamellar spatial organization, which significantly improves light transmittance and distribution, crucial for maximizing the efficiency of photosynthetic reactions. The biomimetic crosslinking strategy, leveraging specific interactions between polyphosphate anions and primary amine groups featured on chitin fibers, produced mechanically robust and wet-resilient cryogels that maintained their functionality under operational conditions. Various model biotransformation reactions leading to value-added chemicals are performed in chitin-based matrix. It demonstrates superior or comparable performance to existing state-of-the-art matrices and suspension-based systems. The findings suggest that chitin-based cryogel approach holds significant promise for advancing the development of solid-state photosynthetic cell factories, offering a scalable solution to improve the efficiency and productivity of light-driven biotransformation.

Phototransposition of Indazoles to Benzimidazoles: Tautomer‐Dependent Reactivity, Wavelength Dependence, and Continuous Flow Studies

Herein, we report a detailed investigation of the photomediated transformation of indazoles to benzimidazoles through a nitrogen‐carbon transposition. This phototransposition is known to occur in low yield when 1H‐indazoles are subjected to high‐energy UVC irradiation. The 2H‐tautomer of indazole absorbs light more strongly than the 1H‐tautomer at longer wavelengths. We leveraged this improved absorbance profile to develop a general system for the high‐yielding conversion of N2‐derivatized indazoles (prepared from the corresponding 1H‐indazoles) to the corresponding benzimidazoles under UVB or UVA irradiation in up to 98% yield. Investigation of the substrate scope revealed a strong correlation between reaction yield and electron density at N2 of the indazole substrate, suggesting the importance of the availability of the lone pair at this position for reaction efficiency. In addition, evaluation of wavelength‐dependent reactivity through the generation of a photochemical action plot revealed that the highest conversion does not only occur at the substrate's maximum absorbance wavelength but also on its red‐side, enabling the use of longer wavelength irradiation to achieve high yields. Building on these insights, a continuous flow protocol was established that enables the phototransposition on preparative scale.

Phototransposition of Indazoles to Benzimidazoles: Tautomer-Dependent Reactivity, Wavelength Dependence, and Continuous Flow Studies.

Herein, we report a detailed investigation of the photomediated transformation of indazoles to benzimidazoles through a nitrogen-carbon transposition. This phototransposition is known to occur in low yield when 1H-indazoles are subjected to high-energy UVC irradiation. The 2H-tautomer of indazole absorbs light more strongly than the 1H-tautomer at longer wavelengths. We leveraged this improved absorbance profile to develop a general system for the high-yielding conversion of N2-derivatized indazoles (prepared from the corresponding 1H-indazoles) to the corresponding benzimidazoles under UVB or UVA irradiation in up to 98% yield. Investigation of the substrate scope revealed a strong correlation between reaction yield and electron density at N2 of the indazole substrate, suggesting the importance of the availability of the lone pair at this position for reaction efficiency. In addition, evaluation of wavelength-dependent reactivity through the generation of a photochemical action plot revealed that the highest conversion does not only occur at the substrate's maximum absorbance wavelength but also on its red-side, enabling the use of longer wavelength irradiation to achieve high yields. Building on these insights, a continuous flow protocol was established that enables the phototransposition on preparative scale.

Preparation and characterization of Pd immobilized on the MIL-125-NH2 as an efficient recyclable metal-organic framework in the Suzuki-Miyaura reaction

In this study, an efficient heterogeneous palladium was developed by modifying the MIL-125-NH2 metal-organic framework bromoacetyl bromide and tetraethylenepentamine ligands. The resulting modified framework was then used as a platform for immobilizing Pd nanoparticles (NPs) to generate the Pd@MIL-125-NH-Ac-TEPA nanocomposite. FT-IR, FESEM, EDS, TEM, CHN, TGA, XRD, and ICP-OES were used to identify the structure of the nanocomposite. The characterization findings approve the formation of well-dispersed Pd nanoparticles with a size distribution of 9 to 23 nm. The Pd@MIL-125-NH-Ac-TEPA nanocomposite with 2.97% loading of Pd exhibited high efficiency in the Suzuki-Miyaura coupling reaction of arylboronic acids with various aryl and heteroaryl halides (chlorides, bromides, and iodides) containing electron-donor and electron-acceptor substituents. The coupling products were obtained in water/ethanol mixture (1:1) as solvent at 60°C for 30 min in 70-99% yields. The nanocatalyst can be recovered easily and reused for at least five consecutive runs without losing its activity significantly. The palladium leaching of the reused nanocatalyst was less than 1%. The results revealed that the introduced nanocatalyst has the potential for other organic transformations.

Visible light-driven copper vanadate/biochar nanocomposite for heterogeneous photocatalysis degradation of tetracycline: Performance, mechanism, and application of machine learning.

Water pollution caused by antibiotics is considered a major and growing issue. To address this challenge, high-performance copper vanadate-based biochar (CuVO/BC) nanocomposite photocatalysts were prepared to develop an efficient visible light-driven photocatalytic system for the remediation of tetracycline (TC) contaminated water. The effects of photocatalyst mass, solution pH, pollutant concentration, and common anions on the TC degradation were investigated in detail. Analytical techniques indicated that the CuVO exhibited a nanobelt-like structure with a uniform distribution on the wrinkled biochar surface. The XRD spectrum confirmed that the as-prepared nanomaterial was composed of Cu3V2O7(OH)2·2H2O. Meanwhile, XPS analysis revealed that copper was present in two forms: monovalent and divalent, while vanadium remained pentavalent. The CuVO/BC exhibited excellent stability and high visible light photocatalytic activity towards TC degradation over a wide pH range. The presence of SO42-, H2PO4-, CO32-, and citric acid inhibited the degradation process due to the consuming of photogenerated h+ and •OH, while Cl- enhanced the efficiency of photocatalytic reactions due to generating chlorine oxidizing species. The CuVO/BC showed lower electron-hole recombination rate, more effective separation of photogenerated carriers, lower charge transfer resistance, and higher visible light absorption capacity comparing to pure CuVO by the addition of BC, thus improving the overall photocatalytic performance. In terms of oxidation mechanism, the EPR test and quenching experiment revealed that the contribution of the active species to the degradation of TC followed the order h+ > 1O2>•OH>•O2-. Through the application of machine learning models to analyse the influencing factors of photocatalytic processes, it was discovered that the GBDT model exhibited optimal reliability for the photocatalytic system, and the simulation results were in agreement with the experimental findings.

Nanoporous high-entropy alloys and metallic glasses: advanced electrocatalytic materials for electrochemical water splitting.

Electrochemical water splitting is a promising approach to convert renewable energy into hydrogen energy and is beneficial for alleviating environmental pollution and energy crises, and is considered a clean method to achieve dual-carbon goals. Electrocatalysts can effectively reduce the reaction energy barrier and improve reaction efficiency. However, designing electrocatalysts with high activity and stability still faces significant challenges, which are closely related to the structure and electronic configuration of catalysts. Nanoporous high-entropy alloys (np-HEAs) and metallic glasses (np-MGs), characterized by long-range chemical disorder intertwined with local chemical order combined with three-dimensional, interconnected nanoporous structure, exhibit distinctive electrocatalytic properties and application potential for electrochemical water splitting. To promote the widespread application of np-HEAs and np-MGs, it is of great significance to rationally design and apply them in the field of electrolytic water splitting. In this review, the basic principles of hydrogen evolution reaction and oxygen evolution reaction as well as the fabrication techniques of np-HEAs and np-MGs are introduced. The recent progress in the efficient application of np-HEAs and np-MGs in electrochemical water splitting, and the current challenges and prospects are summarized. This review will provide theoretical guidance for the development of np-HEAs and np-MGs in electrochemical water splitting applications.