Advanced oxygen carrier plays a pivotal role in various chemical looping processes, such as CO₂ splitting. However, oxygen carriers have been restricted by deactivation and inferior oxygen transferability at low temperatures. Herein, we design an Fe–O_v–Ce–triggered phase-reversible CeO_2−x·Fe·CaO ↔ CeO₂·Ca₂Fe₂O₅ oxygen carrier with strong electron-donating ability, which activates CO₂ at low temperatures and promotes oxygen transformation. Results reveal that the maximum CO₂ conversion and CO yield obtained with 50 mol% CeO_2−x·Fe·CaO are, respectively, 426% and 53.6 times higher than those of Fe·CaO at 700°C. This unique multiphase material also retains exceptional redox durability, with no obvious deactivation after 100 splitting cycles. The addition of Ce promotes the formation of the Fe–O_v–Ce structure, which acts as an activator, triggers CO₂ splitting, and lowers the energy barrier of C═O dissociation. The metallic Fe plays a role in consuming O²⁻_lattice transformed from Fe–O_v–Ce, whereas CaO acts as a structure promoter that enables phase-reversible Fe⁰ ↔ Fe³⁺ looping.

The exsolution method has garnered significant attention owing to its high efficacy in developing highly efficient and stable metal nanocatalysts. Herein, a versatile exsolution approach is developed to embed size-tunable metal nanocatalysts within a conductive metal pnictogenide matrix. The gas-phase reaction of Ru-substituted Ni–Fe-layered-double-hydroxide (Ni₂Fe_1−xRu_x-LDH) with pnictogenation reagents leads to the exsolution of Ru metal nanocatalysts and a phase transformation into metal pnictogenide. The variation in reactivity of pnictogenation reagents allows for control over the size of the exsolved metal nanocatalysts (i.e., nanoclusters for nitridation and single atoms for phosphidation), underscoring the effectiveness of the pnictogenation-driven exsolution strategy in stabilizing size-tunable metal nanocatalysts. The Ru-exsolved nickel–iron nitride/phosphide demonstrates outstanding electrocatalyst activity for the hydrogen evolution reaction, exhibiting a smaller overpotential and higher stability than Ru-deposited homologs. The high efficacy of pnictogenation-assisted exsolution in optimizing the performance and stability of Ru metal nanocatalysts is ascribed to the efficient interfacial electronic interaction between Ru metals and nitride/phosphide ions assisted by the inner sphere mechanism. In situ spectroscopic analyses highlight that exsolved Ru single atoms facilitate more efficient electron transfer to the reactants than the exsolved Ru nanoclusters, which is primarily responsible for the superior impact of the phosphidation-driven exsolution approach.

Cd-based Cs₇Cd₃Br₁₃ perovskites, featuring both tetrahedral and octahedral polyhedral structures, have garnered significant acclaim for their efficient luminescent performance achieved through multi-exciton state regulation by doping. However, it remains controversial whether the doping sites are in the octahedra or tetrahedra of Cs₇Cd₃Br₁₃. To address this, we introduced Pb²⁺ and Sb³⁺ ions and, supported by experimental and theoretical evidence, demonstrated that these ions preferentially occupy the octahedra. Among them, Pb²⁺ ions single doping achieves a near-unity photoluminescence quantum yield of 93.7%, which results in excellent X-ray scintillation performance, high light yield of 41,772 photon MeV⁻¹, and a low detection limit of 29.78 nGy_air s^–1. Moreover, this incorporation of Pb²⁺ and Sb³⁺ enabled an exciton state regulation strategy, resulting in standard white light emission with CIE chromaticity coordinates of (0.33, 0.33). Additionally, a multifaceted optical anticounterfeiting and information encryption scheme was designed based on the differences in optical properties caused by the different sensitivities of [PbBr₆]⁴⁻ octahedron and [SbBr₆]³⁻ octahedron to temperature and excitation wavelengths. These diverse photoluminescence characteristics provide new insights and practical demonstrations for advanced X-ray imaging, lighting, optical encryption, and anticounterfeiting technologies.

Metal halide perovskites exhibit excellent absorption properties, high carrier mobility, and remarkable charge transfer ability, showcasing significant potential as light harvesters in new-generation photovoltaic and optoelectronic technologies. Their development has seen unprecedented growth since their discovery. Similar to metal halide perovskite developments, perovskite quantum dots (PQDs) have demonstrated significant versatility in terms of shape, dimension, bandgap, and optical properties, making them suitable for the development of optoelectronic devices. This review discusses various fabrication methods of PQDs, delves into their degradation mechanisms, and explores strategies for enhancing their performance with their applications in a variety of technological fields. Their elevated surface-to-volume ratio highlights their importance in increasing solar cell efficiency. PQDs are also essential for increasing the performance of perovskite solar cells, photodetectors, and light-emitting diodes, which makes them indispensable for solid-state lighting applications. PQDs' unique optoelectronic characteristics make them suitable for sophisticated sensing applications, giving them greater capabilities in this field. Furthermore, PQDs' resistive switching behavior makes them a good fit for applications in memory devices. PQDs' vast potential also encompasses the fields of quantum optics and communication, especially for uses like nanolasers and polarized light detectors. Even though stability and environmental concerns remain major obstacles, research efforts are being made to actively address these issues, enabling PQDs to obtain their full potential in device applications. Simply put, understanding PQDs' real potential lies in overcoming obstacles and utilizing their inherent qualities.

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.

Photoreforming of formic acid (FA) represents a compelling technology for green hydrogen (H₂) production, but the application is limited by the relatively low activity and selectivity. Recent advancements have introduced transition-metal nitrides (TMNs) as a new class of co-catalysts for photocatalytic FA reforming, showing impressive performance but still having the disadvantage of suboptimal H₂ selectivity. Here, we present a novel Cu–W₂N₃ cocatalyst with abundant Cu single-atom sites. On combining with a CdS photocatalyst, the CdS/Cu–W₂N₃ system demonstrated an elevated H₂ generation rate of 172.69 μmol·h⁻¹ and superior H₂ selectivity in comparison to CdS/W₂N₃. Comprehensive experimental and theoretical investigations indicate that the introduction of Cu single-atom sites in Cu–W₂N₃ leads to a robust interaction with CdS, which optimizes the charge transfer. More significantly, the Cu single-atom sites modify the inert surface of the W₂N₃ cocatalyst, creating conducive electron transfer channels and leading to an abundance of active sites favorable for hydrogen evolution reaction (HER), consequently resulting in higher H₂ selectivity than pristine W₂N₃. This study provides a promising approach to achieving an efficient photoreforming reaction with specific selectivity via the design of novel cocatalysts with specialized active sites.

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.

Sodium-ion batteries have emerged as promising candidates for next-generation large-scale energy storage systems due to the abundance of sodium resources, low solvation energy, and cost-effectiveness. Among the available cathode materials, vanadium-based sodium phosphate cathodes are particularly notable for their high operating voltage, excellent thermal stability, and superior cycling performance. However, these materials face significant challenges, including sluggish reaction kinetics, the toxicity of vanadium, and poor electronic conductivity. To overcome these limitations and enhance electrochemical performance, various strategies have been explored. These include morphology regulation via diverse synthesis routes and electronic structure optimization through metal doping, which effectively improve the diffusion of Na⁺ and electrons in vanadium-based phosphate cathodes. This review provides a comprehensive overview of the challenges associated with V-based polyanion cathodes and examines the role of morphology and electronic structure design in enhancing performance. Key vanadium-based phosphate frameworks, such as orthophosphates (Na₃V₂(PO₄)₃), pyrophosphates (NaVP₂O₇, Na₂(VO)P₂O₇, Na₇V₃(P₂O₇)₄), and mixed phosphates (Na₇V₄(P₂O₇)₄PO₄), are discussed in detail, highlighting recent advances and insights into their structure–property relationships. The design of cathode material morphology offers an effective approach to optimizing material structures, compositions, porosity, and ion/electron diffusion pathways. Simultaneously, electronic structure tuning through element doping allows for the regulation of band structures, electron distribution, diffusion barriers, and the intrinsic conductivity of phosphate compounds. Addressing the challenges associated with vanadium-based sodium phosphate cathode materials, this study proposes feasible solutions and outlines future research directions toward advancement of high-performance vanadium-based polyanion cathodes.

Photothermal catalysis utilizing the full solar spectrum to convert CO₂ and H₂O into valuable products holds promise for sustainable energy solutions. However, a major challenge remains in enhancing the photothermal conversion efficiency and carrier mobility of semiconductors like Bi₂MoO₆, which restricts their catalytic performance. Here, we developed a facile strategy to synthesize vertically grown Bi₂MoO₆ (BMO) nanosheets that mimic a bionic butterfly wing scale structure on a biomass-derived carbon framework (BCF). BCF/BMO exhibits high catalytic activity, achieving a CO yield of 165 μmol/(g·h), which is an increase of eight times compared to pristine BMO. The wing scale structured BCF/BMO minimizes sunlight reflection and increases the photothermal conversion temperature. BCF consists of crystalline carbon (sp²-C region) dispersed within amorphous carbon (sp³-C hybridized regions), where the crystalline carbon forms “nano-islands”. The N–C–O–Bi covalent bonds at the S-scheme heterojunction interface of BCF/BMO function as electron bridges, connecting the sp²-C nano-islands and enhancing the multilevel built-in electric field and directional trans-interface transport of carriers. As evidenced by DFT calculation, the rich pyridinic-N on the carbon nano-island can establish strong electron coupling with CO₂, thereby accelerating the cleavage of *COOH and facilitating the formation of CO. Biomass waste-derived carbon nano-islands represent advanced amorphous/crystalline phase materials and offer a simple and low-cost strategy to facilitate carrier migration. This study provides deep insights into carrier migration in photocatalysis and offers guidance for designing efficient heterojunctions inspired by biological systems.

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.

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.

Development of high-efficiency bifunctional oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) electrocatalysts is vital for the widespread application of zinc–air batteries (ZABs). However, it still remains a great challenge to avoid the inhomogeneous distribution and aggregation of metal single-atomic active centers in the construction of bifunctional electrocatalysts with atomically dispersed multimetallic sites because of the common calcination method. Herein, we report a novel catalyst with phthalocyanine-assembled Fe-Co-Ni single-atomic triple sites dispersed on sulfur-doped graphene using a simple ultrasonic procedure without calcination, and X-ray absorption fine structure (XAFS), aberration-corrected scanning transmission electron microscopy (AC-STEM), and other detailed characterizations are performed to demonstrate the successful synthesis. The novel catalyst shows extraordinary bifunctional ORR/OER activities with a fairly low potential difference (ΔE = 0.621 V) between the OER overpotential (E_j10 = 315 mV at 10 mA cm⁻²) and the ORR half-wave potential (E_half-wave = 0.924 V). Moreover, the above catalyst shows excellent ZAB performance, with an outstanding specific capacity (786 mAh g⁻¹), noteworthy maximum power density (139 mW cm⁻²), and extraordinary rechargeability (discharged and charged at 5 mA cm⁻² for more than 1000 h). Theoretical calculations reveal the vital importance of the preferable synergetic coupling effect between adjacent active sites in the Fe-Co-Ni trimetallic single-atomic sites during the ORR/OER processes. This study provides a new avenue for the investigation of bifunctional electrocatalysts with atomically dispersed trimetallic sites, which is intended for enhancing the ORR/OER performance in ZABs.