The operational efficiency of membrane electrode assemblies in direct liquid fuel cells is critically dependent on the fuel purity in the anode compartment. To address the inherent challenge of fuel mixing problem in alcohol systems, we propose a rational catalyst design strategy focusing on morphological and compositional optimization. Sodium borohydride-derived PtCuMo alloy aerogels (AA) exhibit abundant grain boundary defects, while solvothermally prepared nanowire arrays (NA) maintain excellent single-crystalline characteristics. Density functional theory calculations demonstrate that engineered grain boundaries can effectively broaden the adsorption energy window for key reaction intermediates, enabling superior adaptability to diverse catalytic pathways. By precisely controlling Cu content, we identified Pt₃Cu₃Mo_0.5 AA as the optimal catalyst configuration, demonstrating 150% enhancement in methanol oxidation reaction activity compared to Pt₃Cu₆Mo_0.5 NA (1.5 vs. 0.6 A·mg_Pt⁻¹) and 17% improvement in ethanol oxidation reaction performance versus Pt₃Cu₁Mo_0.5 NA (0.82 vs. 0.70 A·mg_Pt⁻¹). Practical application testing using gas diffusion electrodes (anode loading: 0.85 mg_Pt·cm⁻²) achieved a mass-specific power density of 14.14 W·g_Pt⁻¹ in 1:1 methanol/ethanol blends, representing a 3.5-fold improvement over commercial Pt/C benchmarks. This work establishes a fundamental framework for developing high-performance, broad-spectrum electrocatalysts in advanced fuel cell systems.

Electrolyzing seawater to produce hydrogen can not only address the issue of freshwater scarcity but also provide an abundant raw material for hydrogen production. However, seawater electrolysis for hydrogen production still faces numerous risks and challenges at present. This study focuses on a systematic investigation of FeNiCo-based high-entropy alloy (HEA) nanocatalysts supported on carbon skeletons. By precisely regulating the morphological structure of the carbon skeleton, a carbon support with a large specific surface area and abundant active sites can be obtained. Simultaneously, the elemental composition of the HEA nanoparticles is adjusted to optimize its seawater electrolysis performance. An energy-saving strategy of coupling the anode sulfur oxidation reaction (SOR) with the cathode hydrogen evolution reaction (HER) is employed to assist seawater electrolysis. In alkaline seawater, at a current density of 10 mA·cm⁻², the overpotential of the HER is only 22 mV, and the overpotential of the oxygen evolution reaction (OER) is 264 mV. It also exhibits excellent performance in acidic seawater. In a two-electrode seawater electrolysis system, an applied voltage of 1.55 V is required to reach a current density of 10 mA·cm⁻². More importantly, when using SOR to assist alkaline seawater electrolysis, the applied voltage is successfully reduced to 0.82 V.

Simultaneous nitrate reduction and sulfide oxidation reactions (NO₃RR and SOR) to generate valuable chemicals represent an appealing strategy for green synthesis; however, the sluggish kinetics seriously hinder their application. Herein, we report that Ni dopants can optimize the electronic structure of MoS₂, which thus favors the adsorption of reactants/intermediates and reduces the corresponding energy barriers. As a result, the designed catalyst shows a maximal Faradic efficiency of 88.4% and a corresponding yield rate of 66.7 μmol·h⁻¹·cm⁻² for NH₃ synthesis, accompanied by a high robustness over 60 h. Besides, it can also trigger the SOR activity with a low potential of 0.105 V vs. reversible hydrogen electrode (RHE) to produce 10 mA·cm⁻², far smaller than that needed for conventional water oxidation (1.545 V vs. RHE). Accordingly, a coupling system with NO₃RR and SOR is constructed for synchronous formation of value-added products on both anode and cathode. This work demonstrates an attractive attempt to construct advanced MoS₂-based catalysts towards electrosynthesis.

The rational design of advanced methanol oxidation reaction (MOR) electrocatalysts can significantly enhance the catalytic activity and performance of direct methanol fuel cells (DMFCs). Herein, the electrocatalysis informatics-assisted design electrocatalysts for MOR is firstly conducted by combining machine learning based on 616 experimental data points with first-principles calculations. Guided by this theoretical insight, a highly disordered PtRuPd alloy aerogel is prepared via a facile one-pot synthetic strategy. The obtained electrocatalyst demonstrates excellent mass activity of 2.42 A·mg_Pt⁻¹ and specific activity of 7.13 mA·cm⁻² for MOR, which is considerably higher than that of most Pt-based catalysts. The self-supported ultrathin anode catalyst layer (~6.3 μm) integrated into a membrane electrode assembly exhibits the mass-specific power density of 92.9 W·g_Pt⁻¹ at 65 °C for DMFC operation, surpassing that of recently reported Pt-based catalysts. This work offers a promising approach to exploring a digitalization and intelligent cross-scale design route for MOR electrocatalysts.

Nitric oxide (NO), which generally originates from vehicle exhaust and industrial flue gases, is one of the most serious air pollutants. In this case, the electrochemical NO reduction reaction (NORR) not only removes the atmospheric pollutant NO but also produces valuable ammonia (NH₃). Hence, through the synthesis and modification of Fe₃C nanocrystal catalysts, the as-obtained optimal sample of Fe₃C/C-900 was adopted as the NORR catalyst at ambient conditions. As a result, the Fe₃C/C-900 catalyst showed an NH₃ Faraday efficiency of 76.5% and an NH₃ yield rate of 177.5 μmol·h^–1·cm^–2 at the working potentials of –0.8 and –1.2 V versus reversible hydrogen electrode (vs. RHE), respectively. And it delivered a stable NORR activity during the electrolysis. Moreover, we attribute the high NORR properties of Fe₃C/C-900 to two aspects: one is the enhanced intrinsic activity of Fe₃C nanocrystals, including the lowering of the energy barrier of rate-limiting step (*NOH→*N) and the inhibition of hydrogen evolution; on the other hand, the favorable dispersion of active components, the effective adsorption of gaseous NO, and the release of liquid NH₃ products facilitated by the porous carbon substrate.

The overuse and ineffective management of plastics have led to significant environmental pollution. Catalytic upcycling into value-added chemicals has emerged as a promising solution. This review provides a comprehensive overview of recent advances in catalytic upcycling, focusing on the cleavage of chemical bonds such as carbon–carbon (C–C), carbon–oxygen (C–O), and carbon–hydrogen (C–H) in plastics. It systematically discusses plastics conversion via electrocatalysis, thermal catalysis, and photocatalysis. Additionally, it explores the conversion of plastics into value-added chemicals and functional polymers. The review also addresses the challenges in this field and aims to offer insights for developing sustainable and effective plastics upcycling technologies.

Elucidation the relationship between electrode potentials and heterogeneous electrocatalytic reactions has attracted widespread attention. Herein we construct the well-defined Mn single-atom (MnSA) catalyst with four N-coordination through a simple thermal pyrolysis preparation method to investigate the electrode potential micro-environments effect on carbon dioxide reduction reactions (CO₂RR) and oxygen reduction reactions (ORR). MnSA catalysts generate higher CO production Faradaic efficiency of exceeding 90% at −0.9 V for CO₂RR and higher H₂O₂ yield from 0.1 to 0.6 V with excellent ORR activity. Density functional theory (DFT) calculations based on constant potential models were performed to study the mechanism of MnSA on CO₂RR. The thermodynamic energy barrier of CO₂RR is lowest at −0.9 V vs. reversible hydrogen electrode (RHE). Similar DFT calculations on the H₂O₂ yield of ORR showed that the H₂O₂ yield at 0.2 V was higher. This study provides a reasonable explanation for the role of electrode potential micro-environments.

The coupling of energy-saving small molecule conversion reactions and hydrogen evolution reaction (HER) in seawater electrolytes can reduce the energy consumption of seawater electrolysis and mitigate chlorine corrosion issues. However, the fabrication of efficient multifunctional catalysts for this promising technology is of great challenge. Herein, a heterostructured catalyst comprising CoP and Ni₂P on nickel foam (CoP/Ni₂P@NF) is reported for hydrazine oxidation (HzOR)-assisted alkaline seawater splitting. The coupling of CoP and Ni₂P optimizes the electronic structure of the active sites and endows excellent electrocatalytic performance for HzOR and HER. Impressively, the two-electrode HzOR-assisted alkaline seawater splitting (OHzS) cell based on the CoP/Ni₂P@NF required only 0.108 V to deliver 100 mA·cm⁻², much lower than 1.695 V for alkaline seawater electrolysis cells. Moreover, the OHzS cell exhibits satisfactory stability over 48 h at a high current density of 500 mA·cm⁻². Furthermore, the CoP/Ni₂P@NF heterostructured catalyst also efficiently catalyzed glucose oxidation, methanol oxidation, and urea oxidation in alkaline seawater electrolytes. This work paves a path for high-performance heterostructured catalyst preparation for energy-saving seawater electrolysis for H₂ production.