ChemSusChem最新文献

Rechargeable zinc–air battery (ZAB) commercialization is hampered by low efficiency at the air cathodes, where sluggish kinetics and different reaction mechanisms for the oxygen evolution reaction (OER) and oxygen reduction reaction (ORR) at charging and discharging state, limit overall performance. Herein, we demonstrate a carbon nanotubes-supported ruthenium–manganese dioxide (Ru–MnO₂/CNTs) as a high-performance bifunctional ZABs catalyst fabricated via in situ growth and cation exchange approach. The catalyst features a hierarchical architecture where the CNTs scaffold serves as the structural backbone, while Ru–MnO₂ solid solution nanosheets with intrinsic bifunctional activity grow conformally on its surface. This CNTs-supported design synergistically enables a low ruthenium loading of 9.1 wt% while promising electrochemical performance. Critically, the catalyst achieves an ORR half-wave potential of 0.84 V, a OER overpotential of 210 mV at 10 mA cm⁻², and a narrow OER/ORR potential gap of merely 0.6 V. When integrated into ZABs, this catalyst exhibits excellent performance, with the peak power density of 156 mW cm⁻², a high specific capacity of 802 mA h g⁻¹, and stable cycling performance exceeding 200 h. Consequently, this work demonstrates a viable strategy for synthesizing cost-effective and highly active bifunctional oxygen electrocatalysts with optimized noble metal utilization.

Rechargeable zinc-iodine batteries (RZIBs) have garnered significant attention owing to their distinct superiorities of low cost, high safety, and high theoretical capacity. However, their large-scale implementation is hindered by several critical challenges, including the polyiodide shuttle effect, uncontrolled Zn dendrite growth, interfacial corrosion issues, and pronounced self-discharge. This review systematically summarizes hydrogel electrolyte-based strategies, with the objectives of suppressing the polyiodide shuttle effect, promoting uniform Zn deposition, enhancing environmental adaptability, facilitating multi-electron iodide conversion, and enabling flexible applications. These efforts are expected to advance the development of high-performance, long-lifespan RZIBs toward practical utilization.

All-perovskite tandem solar cells (TSCs) have recently surpassed the 30% power conversion efficiency milestone, positioning mixed tin–lead (Sn–Pb) perovskite as indispensable narrow-bandgap absorbers. Their optimal bandgap, reduced lead content, and solution processability make them promising for next-generation photovoltaics. However, their widespread application is hindered by severe stability issues, primarily the facile oxidation of Sn²⁺ and crystallization mismatch between Sn- and Pb-based phases. Distinct from existing reviews, this short review provides an integrated framework for the two fundamental bottlenecks of Sn–Pb perovskite—Sn²⁺ oxidation and Sn/Pb crystallization mismatch—linking mechanistic insights across precursor chemistry, thin-film formation, and device operation. We summarize recent advances that enable efficiencies >23% together with thousand-hour operational stability, and we outline future directions toward fully integrated, scalable, and commercialization-relevant stability solutions.

Developing sustainable routes to biodegradable polymers from renewable feedstocks is key to reducing reliance on petroleum and mitigating environmental pollution. Amino acids, such as L-alanine, are valuable monomers for biodegradable nylons. Artificial photosynthesis has recently been applied to amino acid synthesis, yet the use of biomass-derived nitrogen sources such as urea in visible-light driven L-alanine synthesis has not yet been explored. Here, we present a novel artificial photosynthetic system that converts urea and pyruvate, both biomass-derived compounds, into L-alanine under visible light. In this system, a visible light-driven NADH regeneration system consisting of triethanolamine (TEOA), zinc meso-tetra(4-sulfonatophenyl)porphyrin tetrasodium salt (ZnTPPS⁴⁻), and pentamethylcyclopentadienyl (Cp*) rhodium 2,2′-bipyridine (bpy) ([Cp*Rh(bpy)(H₂O)]²⁺) is integrated with urease (URE), hydrolyzes urea into ammonia, and L-alanine dehydrogenase (AlDH), catalyzes the reductive amination of pyruvate. Under irradiation, the system produced 0.85 mM L-alanine after 24 h (85% yield based on pyruvate). This work represents the first exploration of urea-based, visible-light powered enzymatic L-alanine synthesis, offering a sustainable route to biodegradable polymer precursors from renewable nitrogen and carbon sources.

This study explores the impact of (i) different installation modes of the molecular rhenium catalyst Re within the PCN-777 metal–organic framework (MOF) and (ii) catalyst loading on the resulting catalytic performance and recyclability of the different hybrid materials in the photocatalytic reduction of CO₂ to CO. Through systematic investigation, we demonstrate that a robust coordination linkage between a zirconium node of the framework and the catalyst, obtained via solvent-assisted ligand incorporation (SALI), minimizes rhenium leaching. In contrast, physical entrapment and electrostatic anchoring methods result in significant rhenium leaching after installation. Additionally, we reveal how the installation mode influences the electronic properties of the catalyst, which allows us to tune the catalytic activity. Furthermore, based on these results, we determine the optimal loading and concentration of Re within the MOF matrix for photocatalytic CO₂ reduction.

Electrocatalytic nitrate reduction reaction (NO₃⁻RR) offers a sustainable and energy-efficient alternative for green ammonia synthesis, with the added benefit of environmental remediation and resource recovery. In recent years, it has attracted significant attention. However, the challenges of achieving high selectivity and maintaining catalyst stability have substantially restricted its practical applications. To address these issues, researchers have proposed a variety of catalytic regulation strategies aimed at enhancing catalyst activity and product selectivity. This review systematically summarizes recent advances in catalyst design for NO₃⁻RR from the perspectives of composition regulation, structural engineering, and support strategies. We highlight the underlying mechanisms and performance features of each strategy, emphasizing their roles in modulating electronic structure, constructing efficient active sites, and optimizing interfacial environments. In addition, we discuss the potential of integrating multiple strategies and deepening the understanding of structure–activity relationships. Finally, we outline future directions and key challenges for developing efficient, stable, and scalable NO₃⁻RR catalytic systems, offering insights to guide continued progress in this emerging field.

With the surging global demand for renewable energy, stimuli-responsive hydrogels have emerged asa research hotspot in this field, owing to their unique stimuli-responsive properties, high water content, and remarkable design flexibility. First, this work systematically introduces the molecular and structural design strategies of stimuli-responsive hydrogels, encompassing diverse stimulus-responsive mechanisms. Subsequently, it comprehensively reviews the application progress of stimuli-responsive hydrogels in emerging energy technologies, including sustainable solar utilization, energy storage and conversion, and intelligent energy management. Additionally, the review analyzes current challenges and explores the future development directions of stimuli-responsive hydrogels in conjunction with sustainable development needs. This review not only comprehensively presents the application potential of stimuli-responsive hydrogels in the new energy field but also provides key references for the subsequent development of high-performance hydrogels and the advancement of renewable energy technologies.

CO₂ electroreduction (CO₂R) using Cu catalysts under acidic conditions currently receives substantial attention as it allows to limit detrimental (bi)carbonate salts formation and precipitation. However, it usually requires high concentrations of K-based electrolytes for suppressing hydrogen evolution (HER) and favoring C₂ products formation. Here we used crown-ethers in order to immobilize alkali cations at the surface of the catalyst and show that this strategy not only allows suppressing HER with much less concentrated electrolyte but also orientates the reaction towards CH₄ formation during acidic CO₂R. The utilization of 10 different crown-ethers allowed to study the effect of the structure of the ligand and the nature of the cation on CO₂R selectivity. The largest Faradic Efficiency for methane (FE_CH4 = 55%) was obtained under an applied current density of −150 mA.cm⁻², using the 4′-amino-benzo-15-crown-5-Na⁺ complex.

Aluminum–sulfur (Al–S) batteries are garnering significant interest as candidates for affordable energy storage systems due to their high theoretical capacity of 1672 mAh g^–1 and the cost-effectiveness of naturally abundant aluminum and sulfur. Nevertheless, challenges such as poor cyclic reversibility and limited practical capacity have resulted in only a few reversibly operating Al–S cells to date. In this study, we introduce an improved Al–S battery configuration by incorporating a novel VN@graphene catalyst into the sulfur cathode in Al–S battery applications. Comprehensive electrochemical tests and ex situ characterizations reveal that, during discharge, the catalyst effectively suppresses the polysulfide shuttle effect through strong adsorption, whereas during charging, it enhances sulfide redox kinetics. Consequently, the modified Al–S cell delivers an initial capacity of approximately 1354 mAh g^–1, maintaining around 507 mAh g^–1 after 200 cycles.

Green hydrogen adoption demands intensive research efforts focusing on improving the performance and durability of electrodes used in water electrolyzers, enabling cheaper hydrogen production on a commercial scale. For catalyzing the oxygen evolution (OER) and hydrogen evolution (HER) electrode reactions in a water electrolyzer, the state-of-the-art electrocatalysts used are expensive and scarce, thus preventing their successful commercialization. There is a dire-need to replace those expensive catalysts with cheaper, earth-abundant non-platinum group of transition metals. Heterointerface engineering could be employed as an effective strategy to synthesize such kind of electrocatalysts to tune the electronic and catalytic properties of these environmentally friendly transition metal electrocatalysts. In this report, we have studied the heterointerface formation between Ni₃S₂ and MnO₂ phases using two synthesis approaches: sequential as well as simultaneous growth methods. Our studies show that sequential growth exhibits a critical impact on the chemical and electrocatalytic behavior of the as-synthesized vertically aligned nanoflakes. When Ni₃S₂ was grown over the MnO₂ phase, it resulted in the most superior bifunctional electrocatalytic activity. Along with the electrical impedance measurement, X-ray photoelectron spectroscopy and Raman spectroscopy reveal that the interfacial charge transfer due to heterointerface formation via sequential growth is more effective than the simultaneous method of heterojunction preparation. The best catalyst exhibits a lowering of OER overpotentials of 300 mV and HER onset overpotentials of 230 mV, surpassing the standard catalysts. DFT study has been performed to correlate the experimental and theoretical reaction kinetics over Ni₃S₂@MnO₂@NF heterointerfaces, which suggests a lower overpotential of 1.391 V when Ni₃S₂ is grown over MnO₂ for OER as compared with the MnO₂ (1.719 V) grown over Ni₃S₂. Ni₃S₂@MnO₂@NF electrodes registered a low cell voltage of 1.68 V at 10 mA cm⁻² current density in an alkaline water electrolysis prototype, performing better than the standard catalyst in terms of cell voltage and operation stability at higher current densities of up to 50 mA cm⁻². This study shows how strategic design of interfaces in heterojunction can control the overall catalytic performance.