The practical application of sulfur-based batteries is significantly limited by sluggish reaction kinetics and structural collapse. Herein, a copper-modified sulfurized polyaniline (CuSPANI) cathode with distinctive d-p-π multi-orbital coupling is constructed through Cu heteroatom introduction. This coupling, arising from hybridization between Cu d orbitals and sulfurized polyaniline (SPANI) p/π orbitals, enables triple electronic modulation: reducing energy barriers to enhance kinetics, expanding electron delocalization to improve conductivity, and activating horizontal Cu d orbitals to strengthen structural stability. Consequently, the aqueous CuSPANI battery delivers a high reversible capacity of 834.75 mAh gs−1 at 3 C and exceptional cycling stability (61.2% capacity retention after 60,000 cycles at 15 C). Moreover, the designed flexible quasi-solid-state pouch cell achieves a 1.25 V output and maintains stable power under deformation, highlighting its potential for wearable energy storage. This work provides new insight into designing high-performance sulfurized polymers via orbital hybridization.
Polyaniline (PANI) modified vanadium oxide nanosheet (VO 2 (B)@PANI) cathodes demonstrate high performance for aqueous zinc-ion batteries (AZIBs).
ABSTRACT Aqueous dual‐ion batteries (DIBs) are becoming one of the most compelling choices for large‐scale stationary energy storage owing to the excellent safety performance, high power density, and cost‐effectiveness. However, their low output voltage leads to insufficient energy density. Here, we design a highly reversible pH‐neutral Ag↔Ag 2 SO 4 electrochemistry and construct a novel Zn‐based conversion‐type aqueous anion–cation shuttle DIB. A dendrite‐free Zn anode with functional graphite layer is prepared to improve cycle life. Benefitting from the synchronous effect of Zn 2+ /SO 4 2− dual charge carries and dendrite‐free anode, the DIB delivers a high output voltage of 1.41 V, volumetric energy density of 3295.4 Wh L −1 at 0.5 A g −1 , and 95.9% capacity retention over 300 cycles at 1 A g −1 , superior to most reported DIBs. As a proof of concept, we fabricate a quasi‐solid‐state aqueous DIB with remarkable mechanical strength, flexibility, and impressive temperature resistance. With working temperature decreasing from 20 to −10°C, it shows only a very low‐capacity loss (8.4%) and negligible polarization change (0.05 V). This work overcomes the bottleneck of low output voltage in aqueous DIBs and offers a promising pathway for the development of future aqueous batteries with high energy density.
WC–W 2 C heterostructures in hierarchically porous N-doped carbon chemically anchor LiPSs and accelerate their conversion,suppressing shuttle effects and improving Li–S battery performance.
Integrating plasmonic metals with wide-band gap semiconductors presents a key challenge in photocatalytic overall water splitting. This integration relies on harnessing four primary physical phenomena: photoelectron generation, surface plasmon resonance (SPR), Schottky barrier height (Phi SBH) modulation, and hot electron transfer. However, the complex interplay of these four mechanisms in advanced photocatalytic systems remains incompletely understood. In this work, a novel and robust photocatalyst was designed, featuring 3D-rGO nanostructures impregnated with gold nanoparticles (AuNPs) deposited onto spheres-on-sphere (SOS) silica coated with TiO2 nanosheets. This design enables a systematic investigation of the relationship among photoelectron generation, SPR effects, Schottky barrier modulation, and hot electron transfer. By synchronizing these phenomena, the 3D-rGO@TiO2@(SOS@AuNPs) photocatalyst achieves high performance and durability in overall water splitting, with hydrogen and oxygen production rates of 244.16 mu mol.h-1.g-1 and 123.07 mu mol. h-1.g-1, respectively. Under the monochromatic light irradiation, the apparent quantum efficiency (AQE) values for the 3D-rGO@TiO2@(SOS@AuNPs) photocatalyst were 11.4 % and 6.1 % under 365 and 530 nm, respectively. Moreover, this photocatalyst maintains high efficiency in various water bases, highlighting its versatility for practical applications. Therefore, this study offers not only a promising synthesis strategy for developing a novel 3D photocatalyst, but also valuable insights into the complex interplay of physical phenomena that drive highly efficient energy conversion.
Lithium-selenium (Li-Se) batteries are considered a promising energy storage alternative, mainly because of the high theoretical volumetric capacity of selenium cathodes. However, the polyselenide shuttle effect, large volume expansion and slow diffusion kinetics during cycling continue to impede their practical application. Herein, we report an enhancement of the Li+ diffusion kinetics via tuning the micropore/mesopore ratio of the chitin-derived hierarchically porous carbon for Li-Se batteries. In this structure, confining Se in the hierarchically porous carbon matrix leads to the direct formation of Li2Se through a solid-solid reaction. The incorporation of the tailored proportion of mesopores provides fast pathways for ion diffusion. This enables rapid electric double layer formation in the micropores, leading to improved rate performance and specific capacity. In addition, the hierarchically porous carbon provides buffer space to mitigate cathode volume changes during cycling. Consequently, the constructed Se@ZnCl2-BPC cathode shows exceptional cycling stability, with an initial capacity of 303.1 mA h g-1 at 2C and a capacity retention of 90.6% after 1000 cycles. As far as we know, this is the first report of engineering porosity for Li-Se batteries. It is believed that our work could underscore the critical importance of the pore ratio of hierarchically porous carbon engineering for developing high-performance Li-Se batteries.
Photocatalytic hydrogen production is a promising strategy for alleviating the energy and environment crises. However, its practical application is still severely limited by insufficient visible-light utilization, the rapid recombination of photogenerated charge carriers and slow surface reaction efficiency. To address these issues, a series of oxygen vacancy-assisted three-dimensionally ordered macroporous (3DOM) TiO2-ZnxCd1-xS composite photocatalysts are designed for enhanced hydrogen production. In this heterojunction structure, the interfaces between TiO2 and ZnxCd1-xS are largely decreased via the in situ formation process to promote the transfer of photogenerated charge carriers. In particular, the extra-generated oxygen vacancies regulate the band structure of the composite photocatalyst to improve the spatial separation of the photogenerated charge carriers. This enables the composite with the Zn/Cd molar ratio of 1 : 1 to achieve a remarkable hydrogen production rate of 20.33 mmol g-1 h-1 and an apparent quantum efficiency (AQY) of 84.5% at 365 nm. By harnessing the synergistic effects of heterojunction and oxygen vacancies, this work provides a novel and effective strategy for designing high-performance photocatalysts for photocatalytic hydrogen production.
Nickel oxide (NiO), owing to its tunable valence states and non-noble-metal cocatalytic properties, has shown great potential in photocatalytic hydrogen evolution. However, challenges remain in achieving highly dispersed loading, precise valence regulation, and optimized interfacial structures. Herein, we establish the Ni0/Ni2+ dual active centers and NiO/TiO2 p-n heterojunction in three-dimensionally ordered macroporous NiOx-TiO2-AH (3DOM NT-AH) composite photocatalyst for photocatalytic hydrogen production. In this unique structure, Ni2+ species are favorable for forming a tightly coupled interfacial p-n heterojunction with TiO2, thereby promoting interfacial charge separation and directional carrier migration, while metallic Ni0 acts as an efficient electron sink and electron-transfer mediator, facilitating rapid electron extraction and transport. Meanwhile, the highly dispersed NiOx nanoparticles are intimately anchored on the 3DOM TiO2 (3DOM T) framework forming p-n heterojunction, further enhancing interfacial electron transfer and suppressing the recombination of photogenerated electron-hole pairs. The synergistic effect of the Ni0/Ni2+ dual active centers and the p-n heterojunction makes that the optimized 3DOM NT-AH sample exhibits excellent photocatalytic hydrogen evolution performance, achieving a hydrogen evolution rate of 3.60 mmol center dot g- 1 center dot h- 1, which is about 16 times that of the unreduced 3DOM NiO-TiO2 (3DOM NT) sample. This work provides a promising strategy for the design of efficient non-noble-metal Ni-based photocatalysts.
Mesoporous carbon materials have emerged as promising candidates for potassium-ion batteries (PIBs) as anode materials due to their tunable pore structure, excellent conductivity, and high surface area. However, the sluggish reaction kinetics caused by the larger radius of K ions results in poor potassium storage performance. Here, we report a facile tetraethyl orthosilicate-mediated co-assembly strategy for anchoring cobalt single atoms into highly nitrogen-doped mesoporous carbon/carbon nanotubes (Co-NMC@CNTs). The resulting composite features large mesopore size of approximately 23.7 nm, robust 1D structure, and abundant active sites introduced by Co single atoms and a high nitrogen doping of 13.6 at.%. Synchrotron radiation analysis and theoretical simulation further demonstrate that the presence of Co single atoms significantly reduces diffusion barriers of K ions and increases energy storage centers. When used as PIB anodes, the newly designed Co-NMC@CNTs electrode demonstrates an exceptional electrochemical performance with a high reversible capacity of 362.3 mAh g-1 at 100 mA g-1 after 300 cycles and an outstanding cycling stability with a capacity of 192.0 mAh g-1 at 1000 mA g-1 after 4000 cycles. This work opens up a new blueprint for achieving high-performance mesoporous carbon-based electrodes in next-generation energy storage applications.
The catalytic efficiency of single-component cobalt catalysts (featuring exclusively Co-based active sites) for styrene epoxidation is significantly constrained by mass-transport limitations inherent to the micropores of conventional supports. To overcome this, we devised a one-stone-two-birds strategy for synthesizing hierarchical CoSAPO-34 using a core-shell ZIF-67@SiO2 composite as a combined Co/Si source and template. This approach simultaneously creates (i) atomically dispersed, high-loading Co(ii) sites within the framework and (ii) a hierarchical pore architecture (micro/meso/macro). The introduced meso/macropores dramatically enhance reactant accessibility to the active sites. This synergistic integration yields exceptional performance in aerobic styrene epoxidation, achieving 95.8% conversion with 70.0% selectivity toward styrene oxide, corresponding to a 67.1% yield in only 4 h at 90 degrees C. The catalytic performance is highly prominent, placing it at a superior level among the monometallic catalysts reported to date for styrene epoxidation, especially given the significantly shorter reaction time required to achieve such high efficiency. This strategy provides a novel blueprint for designing efficient catalysts demanding maximized active-site accessibility.
Lithium-selenium (Li-Se) batteries have garnered significant attention recently due to their high energy density. However, selenium cathodes still face challenges such as poor conductivity and severe volume expansion. In this study, we designed a novel two-dimensional nitrogen-doped lamellar porous carbon/selenium composite cathode material (Se@NLPC-P) for high performance Li-Se batteries. Our results show that the lamellar structure assembled from biomass-derived stacked nitrogen-doped carbon nanosheets possesses a high specific surface area (923 m2 g-1), hierarchically micro/mesoporous structure, and high selenium loading (63.3 wt%), enabling strong anchoring capability for selenium species and accelerated ion/electron transport. Consequently, the Se@NLPC-P cathode retains a reversible capacity of 578 mAh g-1 at 0.5 C after 500 cycles, exhibiting superior rate performance and rapid reaction kinetics. This design of biomass-derived lamellar porous carbon hosts via a molecular structure-directing strategy provides new insights for enhanced performance of Li-Se batteries.
In this study, titanium mesh supported dendritic platinum(Pt) branch catalyst(Pt-x/Ti ) was synthesized by an in situ electrodeposition method for the efficient butadiene selective hydrogenation, which is driven by electricity with water as the source of intermediate hydrogen [H]. It shows that the Pt/Ti with 1200 s of electrodeposition (Pt-1200s/Ti) has a superior performance at a current density of-6.25 mA/cm(2), reaching a butadiene conversion rate of 73% and a target product Faraday efficiency exceeding 75% after 8 h of time on stream. Further analysis reveals that, at current density below 6.25 mA/cm(2), butadiene preferentially adsorbs and reacts with the [H] to form butene with high selectivity; with an increase of current density to 6.25-10 mA/cm(2), the excessive [H] drives the reaction toward over-hydrogenation of butene, leading to decreased selectivity; moreover, at current density above 10 mA/cm(2), partial [H] atoms are combined to H 2 gas, leading to a significant decrease in the Faraday efficiency. This study provides a direction for designing highly stable, selective olefin hydrogenation electrocatalysts.
Zinc ferrite (ZnFe2O4) has gained increasing attention as a visible light-responsive and magnetically recoverable photocatalyst for emerging contaminant degradation. However, its low surface area and rapid charge recombination limit its photocatalytic efficiency. Coupling ZnFe2O4 with other semiconductors has led to zinc ferrite-based heterojunction photocatalysts (ZFHPs), where the heterojunction type and component ratio strongly influence charge-transfer pathways and photocatalytic performance. This review provides an integrated analysis of ZFHPs, emphasizing synthesis strategies from hydrothermal and coprecipitation routes to scalable microwave and combustion methods, as well as structural, optical, electronic, and magnetic characterization techniques that confirm heterojunction formation and interfacial band alignment. In addition to material design, particular attention has been given to dual photocatalytic and photo-Fenton mechanisms, optimization through statistical modeling, performance under solar and LED irradiation, and evaluations in real water matrices that reveal both resilience and limitations under complex conditions. Reusability and regeneration strategies are critically assessed, highlighting the roles of magnetic recovery, thermal and solvent-based treatments, and design approaches to mitigate photo-corrosion and leaching. Finally, prospects for advancing ZFHPs through micro- and millifluidic synthesis for scalable production, in situ characterization to probe interfacial charge dynamics, and evaluation in multi-contaminant systems that better reflect environmental reality are discussed. By integrating these aspects, this review identifies pathways to translate ZFHPs from laboratory demonstrations to practical and sustainable water treatment technologies.
ABSTRACT Aqueous Zn–S batteries (AZSBs) have garnered significant attention owing to their high energy density and low cost. However, their practical application is hindered by the limited electrochemical reversibility of sulfur cathode and the interfacial instability of zinc anode. Here, we developed a functionalized co‐solvent electrolyte incorporating aprotic polar tetramethylurea (TMU) and potassium iodide (KI) as synergistic additives, where TMU regulates the Zn 2+ coordination environment and cooperates with iodide species to construct an electrolyte‐derived, interface‐confined, and coordination‐mediated dynamic ion bridge pathway. This pathway couples TMU‐regulated Zn 2+ transport with I 3 − /I − ‐mediated charge transfer at the sulfur cathode interface, thereby reducing the kinetic barriers for Zn 2+ transport and ZnS conversion. Meanwhile, the TMU/KI‐regulated interfacial environment homogenizes Zn 2+ flux at the anode, promotes uniform Zn plating/stripping, and suppresses parasitic reactions. Through the synergistic regulation of the ion bridge, the AZSB delivers a high specific capacity of 759 mAh g −1 at 5 A g −1 and maintains over 71.2% capacity retention after 1000 cycles. This work proposes a promising electrolyte design strategy for energetic AZSBs via synergistic regulation, offering a promising route toward next‐generation sustainable energy storage systems.
Propane dehydrogenation (PDH) for producing propylene shows great promise owing to its non-oil-based process. Platinum-based catalysts are the commercial choices, however, with the challenge of long-term stability due to the facile Pt sintering at elevated operation temperatures (i.e., >600 degrees C). Herein, confining Pt clusters to CeO2 nano-islands supported on carbon nanotubes (CNT) is developed through an electrostatically driven selective adsorption for achieving a sintering-resistant Pt catalyst with efficient PDH performance. The obtained Pt-CeO2/CNT catalyst (i.e., Pt/CeO2 mass ratio similar to 1:11) shows an unprecedented catalytic PDH performance superior to Pt/CNT, with similar to 40% propane conversion and >90% propylene selectivity at below 470 degrees C. Remarkably, it has an ultralow deactivation rate of 0.006 h(-1), which is 3 times lower than that of Pt/CNT (i.e., 0.02 h(-1)). In-depth analysis reveals that CeO2 nano-islands not only confine Pt sites from sintering by a physical segregation, but also promote a facile desorption of propylene by a strong Pt-CeOx interaction. The oxygen species in CeO2 induce a tandem redox reaction with the H-2 from propane dehydrogenation, shifting the PDH balance to an elevated propane conversion. Moreover, the Pt delta+ active site raised by a moderate Pt-CeO2 interaction was identified as the active site for the excellent PDH performance. Further verification by various oxides as the nano-islands for confining Pt, the strategy shows a universality for developing efficient Pt-based catalysts that operate at low temperature in propane dehydrogenation.
Lithium-selenium (Li-Se) batteries have emerged as a promising alternative for energy storage, primarily due to the high theoretical volumetric capacity of selenium cathodes. However, their practical application is still impeded by the polyselenides shuttle effect, large volume expansion and slow diffusion kinetics during cycling. Herein, we report enhancing the Li+ diffusion kinetics via regulating the porosity of the chitin-derived hierarchically porous carbon for Li-Se batteries. In this structure, Se is confined within the micropores of the conductive porous carbon matrix to promote the formation of the Li2Se through a solid-solid reaction. The incorporation of the tailored proportion of mesopores provides fast pathways for ions diffusion. This enables rapid electric double layer formation in the micropores, resulting in enhanced specific capacity and rate performance. In addition, the incorporated porous carbon provides buffer space to mitigate cathode volume changes during cycling. Consequently, the constructed Se@ZnCl2-BPC cathode exhibits exceptional cycling stability, delivering an initial capacity of 303.1 mAh g⁻¹ at 2C and retaining 90.6% of the capacity after 1000 cycles. To the best of our knowledge, this is the first time to report the regulating porosity for Li-Se batteries. It is believed that this work could underscore the critical importance of the ratio of microporous and mesoporous carbon engineering for developing high-performance Li-Se batteries.
Efficient solar light harvesting is essential for high-performance photocatalysts. Here, Rigorous Coupled-Wave Analysis (RCWA) computational method is used to investigate and optimize the optical absorption of TiO2-BiVO4 inverse opal (IO) structures under varying light incidence angles and pore-filling medium (air or water). Simulations were validated against experimental reflectance data. They revealed that small-pore IOs strongly absorb in the UV-C and UV-B regions due to the slow photon effect, making them ideal for sterilization and water disinfection. Medium- and large-pore IOs benefit from additional slow photon effect at the 2nd order photonic band gap, enhancing absorption across both UV and visible regions. Medium-pore IOs are suited for indoor air treatment and water purification, while large-pore IOs with the highest photon flux enhancement enable solar-driven photocatalysis such as outdoor pollutant removal and hydrogen production. For all tested IO designs, the absorbed photon flux exceeds that of equivalent planar slabs, highlighting the advantage of photonic structuring for sustainable photocatalytic applications.
Lithium-nitrogen (Li-N-2) batteries offer a unique electrochemical paradigm that combines intrinsically safe energy storage with sustainable N-2 conversion to value-added chemicals. About ten years after the first ground-breaking report, the practical development of Li-N-2 batteries is still restricted by poor reversibility and limited cycling stability. Here, we first introduce this highly innovative and promising Li-N-2 battery technology and then specify the key challenges ahead for the poor reversibility of Li-N-2 batteries from reaction mechanisms, characterization technologies, and the battery configurations. We further highlight a flow field-assisted "flow-type" cell configuration that presents exciting future opportunities to realize reversible Li-N-2 batteries. Besides, we discuss that the diversity in terms of electrolytes, electrode materials, and separators is key to establishing long-term Li-N-2 batteries. The possible mechanistic pathways of N-2 reduction and lithiation over heterogeneous electrocatalysts are also discussed. We recommend a rigorous experimental protocol for evaluating Li-N-2 batteries to ensure reproducibility and reliable performance comparison across studies. Overall, this perspective aims to inspire future generations of researchers to advance both fundamental understanding and practical breakthroughs, thereby engineering a paradigm shift in Li-N-2 chemistry research.