The strategy of enhancing biocatalytic activity through the modification of natural cells with nanomaterials has overcome the intrinsic catalytic bottlenecks of bacteria, making significant contributions to energy production and pollution treatment. However, chemically engineered biocatalyst systems remain in their early stages of development. Herein, we report a simple and straightforward strategy for constructing an efficient biocatalyst by incorporating carbon quantum dots (CDs) into Escherichia coli (E. coli) to enhance the oxygen reduction reaction (ORR) at the cathode of microbial fuel cells (MFCs). The introduction of CDs significantly accelerates extracellular electron transfer and metabolic activity, markedly increases intracellular adenosine triphosphate (ATP) levels, and promotes substrate utilization. Furthermore, the engineered E. coli exhibits enhanced surface adhesion and increased electronegativity. Electrochemical measurements demonstrate superior ORR activity, delivering a maximum current density of 3.1 mA·cm−2 and an onset potential of 0.67 V, outperforming many previously reported biocatalysts. When applied in an MFC system, the modified biocatalyst achieves a maximum power density of 325 μW·cm−2, placing it among the highest-performing systems reported to date. This work provides a facile and cost-effective approach for improving MFC performance and offers a promising design strategy for next-generation biohybrid catalysts.

Improving the sluggish ion/electron kinetics of niobium-based oxides is of great significance for the development of extremely fast-charging batteries. Herein, we propose an elemental halogen engineering strategy to tune the oxygen vacancy gradient, thereby tailoring the electronic structure. The Br-TNO-350 exhibited remarkable lithium-ion storage capabilities along with outstanding cycling stability. At 10C, the initial discharge capacity reached 164.71 mAh g−1, and was sustained at 143.26 mAh g−1 after 1000 cycles, reflecting a capacity retention of 86.98%. Even under low-temperature conditions (−10 °C), Br-TNO-350 maintained an average capacity of 73.52 mAh g−1 after 500 cycles at 5C. The improvement can be attributed to the expansion of layer spacing and the creation of oxygen vacancies after doping with Br, which facilitates the transfer of ions and electrons. This research presents a promising strategy to enhance the electrochemical performance of TiNb₂O₇ and provides valuable insights for the development of fast-charging batteries with long cycling life.

Microbial fuel cells (MFCs) have garnered significant attention in recent years as an emerging technology for simultaneous energy recovery and wastewater treatment. However, their practical application remains limited by slow oxygen reduction reaction (ORR) kinetics at the cathode, as well as the high cost and poor environmental compatibility of conventional catalysts. To address these challenges, this study designed a self-supported spongelike porous carbon nanofiber electrode based on microbial electrochemical characteristics. By incorporating a macroporous sponge structure with microporous fiber networks and cultivating a uniform ORR-active biofilm on its surface, a sustainable biocathode is developed for constructing high-performance MFCs. The electrode material (SPCNF@CNT) was fabricated via electrospinning using polyvinyl alcohol-coated carbon nanotubes. Through optimization of fiber morphology, electrical conductivity, and mass transfer properties, the SPCNF@CNT biocathode demonstrated exceptional ORR activity, achieving a current density of 5.13 mA center dot cm-2 and an onset potential of 0.68 V. When applied as an MFC cathode, the system delivered a maximum power density of 378 mu W center dot cm-2 and degraded 19.75 mM of glucose within 90 h, indicating remarkable pollutant removal capacity. This work presents an efficient and stable biocathode system, offering a new strategy to enhance MFC cathode performance and promote its practical implementation.

Aqueous zinc metal batteries are promising for grid energy storage; however, their application is hindered by the irreversibility of Zn chemistry. Electrolyte additives have been demonstrated to be effective in improving Coulombic efficiency (CE), yet the incomplete understanding of the interplay between additives and Zn metal anode (ZMA) is an obstacle to advancing electrolytes. Herein, we propose and validate a molecular design strategy based on two critical factors, dipole moment and isotropic polarizability, which characterize the dynamic nature of additive molecules at the charged interface between ZMA and electrolyte. This design guideline inspires an exemplar molecule, choline glycerophosphate (GPC), to be used as an additive in aqueous ZnCl2 electrolyte. The ZnCl2+GPC electrolyte achieves a high CE of 99.9 % for Zn plating/stripping. The comprehensive analysis of ZMA/electrolyte interface reveals a dynamic interplay mode that is responsible for the excellent reversibility. The high dipole moment and isotropic polarizability of GPC enable it to adsorb on ZMA surface during both charge and discharge processes, while the water reduction is greatly inhibited. The application of ZnCl2+GPC electrolyte is demonstrated in Zn||NH4V4O10 cells at room and sub-zero temperatures. This molecular engineering strategy facilitates the rational design of electrolytes and can be extended to other aggressive alkali-metal batteries.

The disordered structure of electrocatalysts exhibits enhanced catalytic activity. The integration of the disordered structure catalyst into the conductive catalyst is an effective strategy for optimizing the properties of the active site, which is beneficial for enhancing the inhibition of the shuttle effect and the redox kinetics of sulfur species. Herein, an amorphous cerium oxide (CeOx) introduced to the surface of nickel phosphides (Ni2P) is prepared to serve as an electrocatalyst and barrier layer in lithium-sulfur batteries for the first time. The appropriate adsorption capacity of Ni2P/CeOx for soluble sulfur species due to the formation of the multi-active adsorbed sites (Ni-S, Ce-S, O-Li) effectively suppress the shuttle effect. The electronic interaction between CeOx and Ni2P achieves the construction of built-in electric field by the bridge effect exerted of O atoms. The enhanced surface wettability, smaller internal resistances and the synergy between the stronger adsorption capacity of Ni2P for LiPSs and the Li2S deposition/decomposition on the CeOx surface accelerate the redox kinetics. The designed Ni2P/CeOx applied as the interlayer exhibits a long cycle stability (capacity decay of 0.03% per cycle after 2000 cycles at 1C) and a higher capacity of 655.3 mAh g-1 after 700 cycles at 0.5C.

Aqueous Zn-metal batteries (AZMBs) performance is hampered by freezing water at low temperatures, which hampers their multi-scenario application. Hydrogen bonds (HBs) play a pivotal role in water freezing, and proton transport is indispensable for the establishment of HBs. Here, the accelerated proton transport modulates the dynamic hydrogen bonding network of a Zn (BF4)2/EMIMBF4 impregnated polyacrylamide/poly (vinyl alcohol)/xanthan gum dual network eutectic gel electrolyte (PPX-ILZSE) for low-temperature AZMBs. The PPX-ILZSE forms more HBs, shorter HBs lifetimes, higher tetrahedral entropy, and faster desolvation processes, as demonstrated by experimental and theoretical calculations. This enhanced dynamic proton transport promotes rapid cycling of HBs formation-failure, and for polyaniline cathode (PANI) abundant redox sites of proton, confers excellent low temperature electrochemical performance to the Zn//PANI full cell. Specific capacities for 1000 and 5000 cycles at 1 and 5 A g-1 were 149.8 and 128.4 mA h g-1 at room temperature, respectively. Furthermore, specific capacities of 131.1 mA h g-1 (92.4% capacity retention) and 0.0066% capacity decay per lap were achieved for 3000 and 3500 laps at-30 and 40 degrees C, respectively, at 0.5 A g-1. Furthermore, in-situ protective layer of ZnOHF nano-arrays on the Zn anode surface to eliminate dendrite growth and accelerate Zn-ions adsorption and charge transfer. (c) 2025 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. and Science Press. All rights are reserved, including those for text and data mining, AI training, and similar technologies.

Aqueous Zn-iodine (Zn-I2) batteries have attracted much attention due to their high theoretical capacity, high safety, and cost-effectiveness. However, the poor electrical conductivity of iodine and shuttling of polyiodide limit the cycling life of Zn-I2 batteries. Herein, a polyiodide host material constructed by a trifluoromethyl-functionalized covalent organic framework (F-COF) is set to regulate the electronic structure and stable polyiodide shuttle. Strong electron-withdrawing trifluoromethyl groups can improve the electrostatic potential and boost adsorption performance. The theoretical results manifest that F-COF has a high adsorption capacity for polyiodide to inhibit the shuttle effect. In situ Raman spectroscopy shows that I3- and I5- are the main form in the I-/I2 conversion process. Therefore, the F-COF loaded with iodine (F-COF-I2) cathode achieves a specific capacity of 197 mAh g-1 at 1C and a Coulombic efficiency higher than 99.5%. In addition, it has a specific capacity of 112 mAh g-1 and can be stably cycled 40,000 times at 50C. Simultaneously, Zn corrosion can be restricted by F-COF due to its polyiodide capture capacity. This work opens up a new avenue for the construction of polyiodide host materials with superior durability and electronic structure.

The main challenges in aqueous Zn metal batteries (AZMBs) are enhancing energy density and cycling life, which require low Zn deposition/stripping overpotential and a stable anode/electrolyte interface. Herein, a hollow mesoporous Na 3 V 2 (PO 4 ) 3 coated with carbon (HMNVP/C) is designed as the Zn anode protective layer (HMNVP/C@Zn). The zincophilic Na 3 V 2 (PO 4 ) 3 with numerous ion channels accelerates Zn 2+ desolvation, while the hollow mesoporous structure promotes rapid Zn 2+ migration through the artificial solid electrolyte interface (ASEI). Diffusion rate differences between the external wall and hollow core lead to Zn 2+ enrichment and flux homogenization at the anode interface. Consequently, the HMNVP/C@Zn symmetric cell achieves an ultralow overpotential of 13.0 mV at 1 mA cm −2 , with stable cycling for over 1200 h at 0.2 mA cm −2 and 0.2 mAh cm −2 without dendrite growth. Additionally, for the first time, the electrochemical process of the zinc anode is decomposed into seven steps, and determine the relaxation time range of Zn 2+ migration in ASEI by in situ electrochemical impedance spectroscopy (EIS) and distribution of relaxation times (DRT) analysis. It is noted that the rapid Zn 2+ migration within the stable HMNVP/C layer significantly reduces the impedance of subsequent zinc crystal growth. This novel design and characterization technique offer valuable insights for preparing advanced ASEI in AZMBs.

Li-ion batteries for electric vehicles and aviation require fast charging, long cycle life, and a wide operating temperature range. However, the lack of anode materials that offer both high capacity and stability at high charging/discharging rates significantly impedes their development. Herein, the introduction of lanthanide with f-Orbital electronic configurations widens the ion transport channels and significantly alters the original electronic structure, leading to a notable improvement in acceleration kinetics. X-ray absorption spectroscopy is employed to depict lanthanide earth elements that can lower lattice strain and accelerate the diffusion of Li+. The Tm0.01-TNO delivers an outstanding specific capacity of 150.9 mAh g-1 at 50 C. Even at low temperatures (-30 °C), Tm0.01-TNO exhibits stable cycling performance with 100% capacity retention over 500 cycles at 1 C. This work demonstrates an enormous promise for scalability in practical low-temperature applications.

Rational structural tuning of carbon materials to enhance active site and achieve high edge-nitrogen doping is crucial for zinc-ion hybrid capacitors. Herein, for the first time, a strategy using g-C3N4 as a self-sacrificial template and KMnO4 as a pore-forming agent synthesizes coal-derived, edge-nitrogen-rich porous carbon sheets (KNPC). Urea thermally condenses to form a 2D g-C3N4 template, providing a layered skeleton and promoting edge-nitrogen doping in the carbon precursor. KMnO4 reacts with carbon to produce potassium salt and manganese oxide can further etching of the carbon materials to generate massive porous structure. Due to the synergistic influence, the obtained KNPC materials possess unique 2D porous nanosheet-like structure, ultrahigh specific surface area (2054.2 m2 g- 1), rich edge nitrogen (7.46 at. %) and oxygen (13.52 at. %) functional groups. The assembled zinc ion hybrid capacitors (ZIHCs) using KNPC as the cathode, zinc foil as the anode achieves a high energy density of 147.9 Wh kg- 1 and excellent electrochemical stability (98.7 % capacity retention after 50,000 cycle tests) in 2 M ZnSO4 aqueous electrolyte. More interestingly, the assembled flexible ZIHCs exhibit superior energy density (137.6 Wh kg- 1) and excellent electrochemical stability (90.1 % capacity retention after 10,000 cycle tests) in ZnSO4/PAM gel.

Designing electrochemical catalysts has become a research hotspot due to their accelerating the polysulfide conversion of the sulfur cathode to inhibit the "shuttle effect" in lithium-sulfur batteries. However, it is still a great challenge to design the heterogeneous selective electrochemical catalyst for inhibiting the "shuttle effect". Herein, nickel cobalt phosphide and cobalt phosphide as the heterogeneous catalyst active sites embedded in the nitrogen-doped hollow carbon nanocages (NiCoP@CoP/NC) are reported, used for multi-step and multi-phase sulfur electrode reaction, and it is found that metal-sulfur d-p hybridization can effectively indicate the intrinsic catalytic activity of metal site. Division of labor and cooperation of the bi-active NiCoP@CoP as heterogeneous catalysts propel the stepwise polysulfide conversion. NiCoP and CoP sites preferentially accelerate the long-chain polysulfide conversion reaction (S 8 =LiPSs) and the short-chain polysulfide conversion reactions (LiPSs =Li 2 S), respectively. Moreover, the hollow and porous N-doped carbon structure can successfully suppress the volume effect and improve the conductivity of the sulfur cathode. The unique design can obtain an effective inhibition of the shuttle effect and rapid electrode reaction. As a result, Li -S batteries demonstrate a high initial capacity of 1063 mAh g -1 and a low-capacity decay of 0.04% per cycle within 10 0 0 cycles. Our work provides a feasible idea for the design of host materials in Li-S batteries. (c) 2024 Published by Elsevier Ltd on behalf of The editorial office of Journal of Materials Science & Technology.

Atomic substitution engineering is considered as effective strategy to activate the basal plane of molybdenum disulfide (MoS2) which has been demonstrated effective catalytic cathode in lithium-sulfur (Li-S) batteries. Rationally designing atomic substitution structure is vital to figure out the origin of catalytic activity in dopedMoS2 based catalytic cathodes. Herein, an "adjacent period, adjacent group" atomic substitution engineering is constructed to investigate the role of foreign atoms in sulfur redox reaction, and reveal the origin of catalytic activity. Theoretical calculations reveal that the real active sites are the S atoms adjacent to the doped atoms. It has been demonstrated that Nb atomic substitution acts as an initiator to trigger a "Domino Effect" of activating the S sites, enhancing the adsorption ability, facilitating the conversion reaction of sulfur species, and accelerating the Li+ diffusion. Enlightened by the theoretical guidance, Nb-doped MoS2 ultrathin nanosheets assembled hollow nanotubes (Mo1-xNbxS2 HNTs) are fabricated as efficient "adsorption-conversion" sulfur hosts, which exhibit high initial discharge capacities (1163 mAh g- 1 at 0.2 C, 971 mAh g- 1 at 0.5 C). An initial capacity of 613 mAh g- 1 could be achieved under high sulfur loading (3.13 mg cm- 2) and lean electrolyte (5.6 mu L mg- 1). This work provides pivotal guidance to design highly efficient catalytic cathodes for advanced Li-S batteries.

Supercapacitors (SCs) are considered promising energy storge systems because of their outstanding power density, fast charge and discharge rate and long-term cycling stability. The exploitation of cheap and efficient electrode materials is the key to improve the performance of supercapacitors. As the battery-type materials, transition metal phosphides (TMPs) possess high theoretical specific capacity, good electrical conductivity and superior structural stability, which have been extensively studied to be electrode materials for supercapacitors. In this review, we summarize the up-to-date progress on TMPs materials from diversified synthetic methods, diverse nanostructures and several prominent TMPs and their composites in application of supercapacitors. In the end, we also propose the remaining challenges toward the rational discovery and synthesis of high-performance TMP electrodes materials for energy storage.

The regulation of the chemical coordination environment in the electrocatalyst can effectively suppress the shuttle effect of sulfur species in lithium-sulfur batteries. However, the mechanism of the atomically dispersed dual metal atom with the coordination of various heteroatoms used as the sulfur cathode catalyst and trapper remains unknown. This study introduces, for the first time, atomically dispersed Co and Mn in-situ immobilized on O, N dual-doped hollow carbon spheres (SACoMn/C-(N, O)) as sulfur host. Experiments combined with density functional theory calculations reveal that the synergy between Co-(N, O) and Mn-(N, O) sites enhances the nucleation/deposition and decomposition capabilities of Li2S. This enhancement is attributed to the anchoring-coupling-conversion behavior of sulfur species on the SACoMn/C-(N, O) surface, which effectively restrains the shuttle effect and facilitates the conversion kinetics. Moreover, the cooperation of dual metal atoms with O, N non-metal atoms embedded in the carbon network structure accelerates electric transport and ion diffusion kinetics. The cathode demonstrates a high initial specific capacity of 890 mAh & sdot;g- 1 at 1 C and show exceptional long-term cycling durability, with a low capacity degradation of 0.037 % per cycle after 1700 cycles. This research may offer novel insights into the design of dual metal atom-decorated, functionalized carbon materials to improve the conversion reaction in sulfur cathodes.

Nano-engineering and hybrid with carbon are effective methods for improving the electrochemical performance of Mn3O4 anodes. However, there are many difficulties in further reducing the size of Mn3O4. To solve these challenges, a novel hollow microsphere structure constituted of ultra-small Mn3O4 nanoparticles (less than 5 nm) embedded within ultrathin carbon nanosheets is designed as anode materials by a simple two-step heating treatment method. The ultra-small Mn3O4 nanoparticles will accelerate the kinetic reaction process and relieve volume variation. Meanwhile, In-situ fabrication of conductive carbon nanosheets play an important role in the electronic/ion transfer and the structure stability. Due to the synergistic effect of ultra-small Mn3O4 nanoparticles and carbon nanosheets, the material shows a topmost reversible capacity of 804 mAh g-1 at the current density of 1 C and maintains a high specific capacity of 603 mAh g-1 after 700 cycles. The strategy can be extended to prepare of other functional nanoparticles and apply in energy storage and catalysis.

TiNb2O7 (TNO) has emerged as a highly potential power-type anodes for extremely fast-charging batteries. Nevertheless, the inherent electron conductivity and crystalline stability of TNO, limiting its actual capacity. Herein, a TNO anode doped by highly oxidized state ions is designed for regulating unit cell volume expansion, oxygen vacancies generation and charge mobility through induced Nb-O bond distortion. The Ce-0.01-TNO electrode shows a high discharge capacity of 181 mAhg(-1) at 20 C after 1000 cycles. Meanwhile, the density functional theory simulations demonstrate that decreased ion-diffusion barrier and increased electronic conductivity are obtained by narrowing the bandgap and introducing impurity bands induced by Ce doping. This work provides an effective strategy to enhance the electrochemical performance of TiNb2O7, making a guideline to construct fast-charging batteries with a prolonged cycle lifespan.

Single-crystal metal foils with high-index facets are currently being investigated owing to their potential application in the epitaxial growth of high-quality van der Waals film materials, electrochemical catalysis, gas sensing, and other fields. However, the controllable synthesis of large single-crystal metal foils with high-index facets remains a great challenge because high-index facets with high surface energy are not preferentially formed thermodynamically and kinetically. Herein, single-crystal nickel foils with a series of high-index facets are efficiently prepared by applying prestrain energy engineering technique, with the largest single-crystal foil exceeding 5×8 cm2 in size. In terms of thermodynamics, the internal mechanism of prestrain regulation on the formation of high-index facets is proposed. Molecular dynamics simulation is utilized to replicate and explain the phenomenon of multiple crystallographic orientations resulting from prestrain regulation. Additionally, large-sized and high-quality graphite films are successfully fabricated on single-crystal Ni(012) foils. Compared to the polycrystalline nickel, the graphite/single-crystal Ni(012) foil composites show more than five-fold increase in thermal conductivity, thereby showing great potential applications in thermal management. This study hence presents a novel approach for the preparation of single-crystal nickel foils with high-index facets, which is beneficial for the epitaxial growth of certain two-dimensional materials.

The design and preparation of bifunctional electrode materials play a vital role in the field of energy storage and conversion. Herein, Mo-doped Ni3S2 nanosheet arrays assembled on nickel foam (named as Mo-Ni3S2) are designed through three-step continuous hydrothermal methods for enhanced hydrogen evolution reaction (HER) and supercapacitor storage characteristics. The ultrathin Mo-Ni3S2 nanosheets structure could modulate electronic structure and offer rich actives sites, thereby expediting the mobility of charge carriers and engendering a greater density of active sites. Consequently, the Mo-Ni3S2 exhibits low overpotential both in alkaline and acidic solution with the value of 53 and 65 mV at the current density of 10 mA cm−2, respectively. Meanwhile, the HER activity can be well maintained after 17 h of continuous operation at 10 mA cm−2, demonstrating its excellent stability. Furthermore, the as-prepared Mo-Ni3S2 as pseudocapacitive materials exhibits a specific capacitance of 3528 F g−1 at 1 A g−1, implying outstanding long durability with 96.5% capacity retention after 3000 charge–discharge cycles. Overall, this work provides a viable strategy for the development of transition metal-based materials as efficient bifunctional catalysts.