Carbon Energy最新文献

All-solid-state batteries (ASSBs) are a promising next-generation energy storage solution due to their high energy density and enhanced safety. To achieve this, specialized electrode designs are required to efficiently enhance interparticle lithium-ion transport between solid components. In particular, for active materials with high specific capacity, such as silicon, their volume expansion and shrinkage must be carefully controlled to maintain mechanical interface stability, which is crucial for effective lithium-ion transport in ASSBs. Herein, we propose a mechanical stress-tolerant all-solid-state graphite/silicon electrode design to ensure stable lithium-ion diffusion at the interface through morphology control of active material particles. Plate-type graphite with a high surface-area-to-volume ratio is used to maximize the dispersion of silicon within the electrode. The carefully designed electrode can accommodate the volume changes of silicon, ensuring stable capacity retention over cycles. Additionally, spherical graphite is shown to contribute to improved rate performance by providing an efficient lithium-ion diffusion pathway within the electrode. Therefore, the synergistic effect of our electrode structure offers balanced electrochemical performance, providing practical insights into the mechano–electrochemical interactions essential for designing high-performance all-solid-state electrodes.

The recovery and utilization of ubiquitous low-grade heat are crucial for mitigating the fossil energy crisis. However, uncontrolled spontaneous heat dissipation limits its practical application. Inspired by skeletal muscle thermogenesis, we develop a compressible wood phase change gel with mechano-controlled heat release by infiltrating xylitol gel into wood aerogel. The xylitol gel can store recovered low-grade heat for at least 1 month by leveraging its inherent energy barrier. The hierarchically aligned lamellar structure of wood aerogel facilitates mechanical adaptation, hydrogen bond formation, and energy dissipation between the wood aerogel and the xylitol gel, increasing the compressive strength and toughness of wood phase change gel fivefold compared to xylitol gel. This enhancement effect enables repetitive contact-separation motions between the wood phase change gel and the substrate during radial compression, overcoming the energy barrier and releasing approximately 178.6 J g⁻¹ of heat. As a proof-of-concept, the wood phase change gel serves as the hot side in a thermoelectric generator, providing about 2.13 W m⁻² of clean electricity by the controlled utilization of recovered solar heat. This study presents a sustainable method to achieve off-grid electricity generation through the controlled utilization of recovered low-grade heat.

The use of conjugated microporous polymers (CMPs) in photocatalytic CO₂ reduction (CO₂RR), leveraging solar energy and water to generate carbon-based products, is attracting considerable attention. However, the amorphous nature of most CMPs poses challenges for effective charge carrier separation, limiting their application in CO₂RR. In this study, we introduce an innovative approach utilizing donor π-skeleton engineering to enhance skeleton coplanarity, thereby achieving highly crystalline CMPs. Advanced femtosecond transient absorption and temperature-dependent photoluminescence analyses reveal efficient exciton dissociation into free charge carriers that actively engage in surface reactions. Complementary theoretical calculations demonstrate that our highly crystalline CMP (Py-TDO) not only greatly improves the separation and transfer of photoexcited charge carriers but also introduces additional charge transport pathways via intermolecular π–π stacking. Py-TDO exhibits outstanding photocatalytic CO₂ reduction capabilities, achieving a remarkable CO generation rate of 223.97 μmol g⁻¹ h⁻¹ without the addition of chemical scavengers. This work lays pioneering groundwork for the development of novel highly crystalline materials, advancing the field of solar-driven energy conversion.

The robustness of single-atom catalysts (SACs) is a critical concern for practical applications, especially for thermal catalysis at elevated temperatures under reductive conditions. In this study, a laser solid-phase synthesis technique is reported to fabricate atom-nanoisland-sea structured SACs for the first time. The resultant catalysts are constructed by Pt single atoms on In₂O₃ supported by Co₃O₄ nanoislands uniformly dispersed in the sea of reduced graphene oxide. The laser process, with a maximum temperature of 2349 K within ~100 μs, produced abundant oxygen vacancies (up to 70.8%) and strong interactions between the Pt single atoms and In₂O₃. The laser-synthesized catalysts exhibited a remarkable catalytic performance towards CO₂ hydrogenation to methanol at 300°C with a CO₂ conversion of 30.3%, methanol selectivity of 90.6% and exceptional stability over 48 h without any deactivation, outperforming most of the relevant catalysts reported in the literature. Characterization of the spent catalysts after testing for 48 h reveals that the Pt single atoms were retained and the oxygen vacancies remained almost unchanged. In situ diffuse reflectance infrared Fourier transform spectrum was conducted to establish the reaction mechanism supported by the density functional theory simulations. It is believed that this laser synthesis strategy opens a new avenue towards rapidly manufacturing highly active and robust thermal SACs.

Considering the growing pre-lithiation demand for high-performance Si-based anodes and consequent additional costs caused by the strict pre-lithiation environment, developing effective and environmentally stable pre-lithiation additives is a challenging research hotspot. Herein, interfacial engineered multifunctional Li₁₃Si₄@perfluoropolyether (PFPE)/LiF micro/nanoparticles are proposed as anode pre-lithiation additives, successfully constructed with the hybrid interface on the surface of Li₁₃Si₄ through PFPE-induced nucleophilic substitution. The synthesized multifunctional Li₁₃Si₄@PFPE/LiF realizes the integration of active Li compensation, long-term chemical structural stability in air, and solid electrolyte interface (SEI) optimization. In particular, the Li₁₃Si₄@PFPE/LiF with a high pre-lithiation capacity (1102.4 mAh g⁻¹) is employed in the pre-lithiation Si-based anode, which exhibits a superior initial Coulombic efficiency of 102.6%. Additionally, in situ X-ray diffraction/Raman, density functional theory calculation, and finite element analysis jointly illustrate that PFPE-predominant hybrid interface with modulated abundant highly electronegative F atoms distribution reduces the water adsorption energy and oxidation kinetics of Li₁₃Si₄@PFPE/LiF, which delivers a high pre-lithiation capacity retention of 84.39% after exposure to extremely moist air (60% relative humidity). Intriguingly, a LiF-rich mechanically stable bilayer SEI is constructed on anodes through a pre-lithiation-driven regulation for the behavior of electrolyte decomposition. Benefitting from pre-lithiation via multifunctional Li₁₃Si₄@PFPE/LiF, the full cell and pouch cell assembled with pre-lithiated anodes operate with long-time stability of 86.5% capacity retention over 200 cycles and superior energy density of 549.9 Wh kg^–1, respectively. The universal multifunctional pre-lithiation additives provide enlightenment on promoting large-scale applications of pre-lithiation on commercial high-energy-density and long-cycle-life lithium-ion batteries.

Hydrogen peroxide (H₂O₂) is an eco-friendly chemical with widespread industrial applications. However, the commercial anthraquinone process for H₂O₂ production is energy-intensive and environmentally harmful, highlighting the need for more sustainable alternatives. The electrochemical production of H₂O₂ via the two-electron water oxidation reaction (2e⁻ WOR) presents a promising route but is often hindered by low efficiency and selectivity, due to the competition with the oxygen evolution reaction. In this study, we employed high-throughput computational screening and microkinetic modeling to design a series of efficient 2e⁻ WOR electrocatalysts from a library of 240 single-metal-embedded nitrogen heterocycle aromatic molecules (M-NHAMs). These catalysts, primarily comprising post-transition metals, such as Cu, Ni, Zn, and Pd, exhibit high activity for H₂O₂ conversion with a limiting potential approaching the optimal value of 1.76 V. Additionally, they exhibit excellent selectivity, with Faradaic efficiencies exceeding 80% at overpotentials below 300 mV. Structure-performance analysis reveals that the d-band center and magnetic moment of the metal center correlated strongly with the oxygen adsorption free energy ($��\; ��{�∆�\; �G�}_{O^{*}}��$), suggesting these parameters as key catalytic descriptors for efficient screening and performance optimization. This study contributes to the rational design of highly efficient and selective electrocatalysts for electrochemical production of H₂O₂, offering a sustainable solution for green energy and industrial applications.

Cu-based metal-organic frameworks (Cu-MOFs) electrocatalysts are promising for CO₂ reduction reactions (CO₂RR) to produce valuable C₂₊ products. However, designing suitable active sites in Cu-MOFs remains challenging due to their inherent structural instability during CO₂RR. Here we propose a synergistic strategy through thermal annealing and electrochemical-activation process for in-situ reconstruction of the pre-designed Cu-MOFs to produce abundant partially oxidized Cu (Cu^δ+) active species. The optimized MOF-derived Cu^δ+ electrocatalyst demonstrates a highly selective production of C₂₊ products, with the Faradaic Efficiency (FE) of 78 ± 2% and a partial current density of −46 mA cm⁻² at −1.06 V_RHE in a standard H-type cell. Our findings reveal that the optimized Cu^δ+-rich surface remains stable during electrolysis and enhances surface charge transfer, leading to an increase in the concentration of *CO intermediates, thereby highly selectively producing C₂₊ compounds. This study advances the controllable formation of MOF-derived Cu^δ+-rich surfaces and strengthens the understanding of their catalytic role in CO₂RR for C₂₊ products.

Front cover image: Practical green hydrogen production requires efficient, low-cost, nontoxic materials integrated into simple device architectures. However, achieving high solar-to-hydrogen (STH) efficiency using solely earth-abundant materials in the overall device remains a critical bottleneck. In article number CEY2706, Park et al. report a solar hydrogen production system with over 10% STH efficiency under unbiased conditions. The device combines a Se-incorporated Ni3S2 electrocatalyst with a ternary bulk heterojunction organic semiconductor composed of PM6, D18, and L8-BO. Ternary absorber enables tailored photovoltage and enhanced photocurrent by suppressing non-radiative decay pathways. Effective integration of the catalyst and light absorber offers a simple and effective route for benchmark-efficiency solar hydrogen production using earth-abundant materials.

Back cover image: Large-scale green hydrogen production technologies play an important role in replacing fossil fuels. However, its cost heavily relies on non-precious metal electrocatalysts with high activity and stability under industrial conditions. In article number CEY2684, Pan et al. fabricated a Fe and Co co-incorporated nickel (oxy) hydroxide exhibits outstanding OER performance under industrial conditions. The surface-reconstructed γ-NiOOH with high valence state is the active layer, where the optimal (Fe, Co) co-incorporation tunes its electronic structure, change the potential determining step, and reduces the energy barrier, leading to ultra-high activity and stability.

Lithium metal is a compelling choice as an anode material for high-energy-density batteries, attributed to its elevated theoretical specific energy and low redox potential. Nevertheless, challenges arise due to its susceptibility to high-volume changes and the tendency for dendritic development during cycling, leading to restricted cycle life and diminished Coulombic efficiency (CE). Here, we innovatively engineered a kind of porous biocarbon to serve as the framework for a lithium metal anode, which boasts a heightened specific surface area and uniformly dispersed ZnO active sites, directly derived from metasequoia cambium. The porous structure efficiently mitigates local current density and alleviates the volume expansion of lithium. Also, incorporating the ZnO lithiophilic site notably reduces the nucleation overpotential to a mere 16 mV, facilitating the deposition of lithium in a compact form. As a result, this innovative material ensures an impressive CE of 98.5% for lithium plating/stripping over 500 cycles, a remarkable cycle life exceeding 1200 h in a Li symmetrical cell, and more than 82% capacity retention ratio after an astonishing 690 cycles in full cells. In all, such a rationally designed Li composite anode effectively mitigates volume change, enhances lithophilicity, and reduces local current density, thereby inhibiting dendrite formation. The preparation of a high-performance lithium anode frame proves the feasibility of using biocarbon in a lithium anode frame.