Rechargeable magnesium-ion batteries (RMBs) demonstrate notable benefits, including higher theoretical energy density, cost-effectiveness, and improved safety characteristics, positioning them as a viable substitute for conventional energy storage solutions. Nevertheless, the ongoing development of high-performance RMBs continues to face inevitable challenges, such as unsatisfactory practical capacity, inadequate cycle durability, swift energy degradation, and a comparatively limited-service life. Herein, CoS/NiS nanomaterials with cubic-shaped morphology were prepared by a two-step metal sulfide template-free solvothermal synthesis method. The material with internal cavity structure effectively mitigates the large expansion of magnesium-ion battery cathode material due to Mg2+ embedding during the charging and discharging process, and provides a robustness electrode-electrolyte interface, thus greatly improving the cycle life. Besides, the introduction of Ni elements into CoS materials may form heterojunctions thereby lowering the potential barrier of the conversion reaction and improving the reaction kinetics and redox reversibility. In addition, the abundance of highly electronegative SS bonds in the CoS/NiS material, which also provides many electrochemically active sites and smooth transport paths for the embedding of Mg2+, leads to the reduction of its polarization and the improvement of its reaction kinetics, which makes the CoS/NiS as a RMBs cathode material with a high specific capacity and a long cycling life. Thus, this research presents a feasible and effective strategy for enhancing the Mg2+ storage capability of engineered CoS nanomaterials, with potential applicability and adaptability to other electrode materials.

Controlling radical selectivity within nanoreactors remains a formidable challenge due to the inherent high reactivity and short half-lives of reactive species. Herein, we report a novel size-matched nanoconfinement strategy using a cobalt-nickel-layered double hydroxide (CoNi-LDH) nanoreactor for the highly selective generation and stabilization of sulfate radicals (SO4 center dot-) via piezoelectric activation of peroxymonosulfate (PMS). By precisely tailoring the LDH interlayer spacing to 5.27 & Aring; to match the kinetic diameter of SO4 center dot-, the nanoreactor effectively suppresses non-selective side reactions and radical quenching. Consequently, the CoNi-LDH achieves an unprecedented reaction rate (kobs = 0.40 min-1) and superior defluorination efficiency (78.9%) for fluoroquinolone antibiotics, significantly outperforming non-size-confined counterparts. Mechanistic insights reveal a synergistic pathway where piezo-generated hot electrons, mediated by Ni sites, accelerate the Co2+/Co3+ redox cycle to ensure long-term catalytic stability. The robustness of this nanoconfined system is further demonstrated by its exceptional tolerance to complex water matrices and its practical operability in a continuous-flow reactor. This study provides a pioneering approach for spatial radical control at the nanoscale to achieve efficient and targeted environmental remediation.

LiMPO4 (M = Fe, Mn) is hydrothermally synthesized in the P-excess reaction system to elucidate the reaction mechanism, and the results unveil that the formation of LiMnPO4 and LiFePO4 has the same reaction mechanism of dissolution-precipitation-ion exchange. Such a composite mechanism contains a key step involving the precipitation of an intermediate during the hydrothermal reaction. This work provides a mechanistic insight into the hydrothermal synthesis of LiMPO4 in a P-excess reaction system, which is fundamentally important for optimal performance.

The persistent organic pollutants in wastewater have caused a heavy threat to ecosystems and humans, but selective removal of these pollutants still faces challenges due to low efficiency, extra addition of oxidation agents, and many highly toxic intermediate products. Herein, we report an efficient, fast kinetic conversion via a photo-self-Fenton-like system of *OOH intermediate-involved oxidation pathway with a high selection generation of singlet oxygen ( 1 O 2 ) from the novel in situ H 2 O 2 heterolytic activation route for the first time. The single-atom and cluster-doped zinc oxide (Ag SA –Ag C /ZnO) was successfully synthesized to achieve the 100% degradation yield and 80% total of carbon (TOC) of the p -chlorophenol (4-CP) as the typical pollutant under solar-light irradiation and exhibit long-term activity in a self-designed photo-Filter reactor for 4-CP degradation. It was attributed to the accelerated cycles from Ag high δ+ site to Ag low δ+ site in Fenton-like catalysis, achieving the rapid selection conversion from the H 2 O 2 heterolytic cleavage to ∼100% 1 O 2 via the intermediate *OOH at the Ag SA sites for ring-opening reaction and reactive H* at the Ag clusters sites for dechlorination reaction, respectively. This discovery gives the deep understanding of the high-performance photo-self-Fenton reaction through in situ cycles of variable metals for the organic contaminants treatment.

Chlorophenols are difficult to degrade and mineralize by traditional advanced oxidation processes due to the strong electronegativity of chlorine. Here, a dual-site atomically dispersed catalyst (Fe-Mo-NC) is reported, which Fe/Mo supported on mesoporous nitrogen-doped carbon is prepared through high-temperature migration. The Fe-Mo-NC exhibits a high dechlorination rate of 93.3% within 1 min. Theoretical calculation suggested that the doping of high-valence Mo6+ as the electron reservoir, promoted electronic delocalization at Fe sites, thereby enhancing the adsorption and dissociation of peroxymonosulfate (PMS), subsequent generation of Fe (IV) = O and singlet oxygen (1O2) species. An interesting finding is that Mo sites can adsorb chlorine sites in 4-chlorophenol (4-CP) and induce C-Cl bond fracture. Thus, the Fe-Mo-NC/PMS system has high catalytic performance due to the synergistic effects of Mo-induced dechlorination and non-radical species (Fe(IV) = O and 1O2) as the degradation pathways, the degradation efficiency of 99.1% of 4-CP within 5 min without significant performance decline after 168 h approximate to 15,120-bed volumes. These findings can advance mechanistic understanding of PMS activation at the molecular level and guide the rational design of efficient eco-friendly single-atom catalysts (SACs) catalysts with bimetallic atomic sites.

The efficient separation of photo-generated electrons and holes is significantly importance for enhancing photocatalytic performance. However, there are few reports on precisely constructing interfaces within a single nanocrystal to investigate the mechanism of photoinduced carrier transfer. In this study, nanorod heterodimer-structured CuS/ZnxCd1−xS heteronanocrystals (CuS/ZnCdS HNCs) were successfully synthesized as a typical model to explore the photoinduced carrier dynamics in the photocatalytic hydrogen evolution reaction (HER). The CuS/ZnCdS HNCs exhibited a photocatalytic hydrogen evolution activity of 146 mmol h⁻1 g⁻1 under visible light irradiation, which is higher than most reported values. Moreover, after 15 h of hydrogen production cycling tests, we found that the material maintained high hydrogen production performance, indicating excellent stability. The CuS/ZnCdS HNCs achieved an apparent quantum yield (AQY) of 69.2% at 380 nm, which is the highest value reported so far for ZnCdS- or CuS-based photocatalysts. The remarkable activity and stability of the CuS/ZnCdS HNCs were attributed to the strong internal electric field (IEF) and Z-scheme mechanism, which facilitate efficient charge separation, as demonstrated by in situ X-ray photoelectron spectroscopy (XPS) and electron paramagnetic resonance (EPR) analyses. This discovery provides a new approach for constructing Z-scheme heterogeneous copper-based nanocomposites within nanocrystals and offers guidance for improving photocatalytic activity.

Toward practical lithium-sulfur (Li-S) batteries, there is a pressing need to improve the rate performance and longevity of cells. Herein, we report developing a cathode electrocatalyst Lu SA/NC, capable of accelerating sulfur redox kinetics with a high specific capacity of 1391.8 mAh g- 1 at 0.1 C, and a low-capacity fading rate of 0.049 % per cycle over 1000 cycles even with a high sulfur loading (5.96 mg cm- 2). The unparalleled cathodes are built upon the unique structure in which single-atoms of rare earth metals are doped in nitrogen-doped porous carbon (RM SAs/NC). The theoretical and experimental studies reveal that the rare earth Lu atom has an unrivaled adsorption capacity for polysulfides and can promote facile deposition and dissolution reactions in charge-discharge processes. The in-situ Raman experiments provide direct evidence for its promotion of polysulfide transformation to eliminate the shuttle effect. The theoretical calculations suggest that the presence of f-dp hybridization enables accelerating sulfur reduction kinetics and enhancing lithium-sulfur battery performance. The strategic paradigm introduced in this study underscores significant practical potential in the exploration of rare earth single-atom catalysts for high performance Li-S batteries.

The fabrication of dual-quantum dot heterostructures offers a promising strategy to enhance the environmental remediation performance of photocatalysts. Herein, a Bi2WO6-based Z-scheme heterojunction was constructed by incorporating carbonized polymer dots (CPDs) and CdS quantum dots (QDs) via a microwave-assisted solvothermal method. The 1 wt% CPDs/CdS QDs/Bi2WO6 (CCBW-1) composite achieved optimal Cr(VI) removal, reaching 97.7 % within 30 min under 10 W LED light, with rate constants 4.4, 2.8, and 10.1 times higher than those of pristine Bi2WO6, CdS QDs/Bi2WO6, and 3 % CPDs/Bi2WO6, respectively. Notably, the composite also demonstrated 96.9 % Cr(VI) and 98.1 % Rhodamine B (RhB) removal within 30 min in a mixed Cr(VI) and RhB solution. The formation of strong Bi-S and W-O-Cd bonds at the Bi2WO6-CdS QD interface facilitates intimate interfacial contacts and creates atomic-scale "highways" that accelerate charge transfer. Additionally, the electron-donating effects of the - NH 2 and - OH functional groups on the CPDs further enhance carrier transfer efficiency. The Z-scheme electron transport pathway enables CCBW-1 to capitalize on the deep reduction potentials and extended light absorption of the dual-QDs, allowing them to act synergistically as active centers. By integrating experimental data with theoretical calculations, the photocatalytic mechanism, potential in- termediates, photodegradation pathway, and biological toxicity were comprehensively elucidated.

The high recombination of photoinduced electron-hole and deep charge trapping in graphitic carbon nitride (gC3N4)-based photocatalysts have limited the photocatalytic activity in hydrogen evolution reaction (HER). Here, we proposed the synergistic strategies of electron-deficient boron (B) and electron-rich phosphorus (P) doped gC3N4 (BPCN) through tuning the electron density for enhanced photocatalytic activity in HER under visible light irradiation. The BPCN exhibited highest photocatalytic activity in HER with the apparent quantum efficiency of 17.4% at 400 nm superior to reported g-C3N4-based photocatalysts. The remarkable activity in HER was attributed to the efficient charge separtion by the shallow charge capture, electron transfer from P to B and the efficient hydrogen spillover pathway occurred by the strong absorption H2O at P sites and then H transferring to B sites. This work paves a new route to changing the electronic density with the tunable band structures through the doping engineering for enhanced photocatalytic activity.

Although photocatalytic hydrogen production from water holds great potential as a renewable and sustainable energy alternative, the practical application of the technology demands cost-effective, simple photocatalytic systems with high efficiency in hydrogen evolution reaction (HER). Herein, the synthesis and characterization of Cu31S16/ZnxCd1-xS heterostructured nanoplates (Cu31S16/ZnCdS HNPs) as a high photocatalytic system are reported. The cost-effective, hierarchical structures are easily prepared using the Cu31S16 NPs as the seed by the epitaxial growth of the ZnCdS nanocrystals (NCs). The Cu31S16/ZnCdS without the noble metal cocatalyst exhibits a high HER rate of 61.7 mmol g(-1) h(-1), which is 8,014 and 17 times higher than that of Cu31S16 and ZnCdS, respectively, under visible light irradiation. The apparent quantum yield (AQY) of Cu31S16/ZnCdS reaches 67.9% at 400 nm with the highest value so far in the reported ZnCdS-based photocatalysts. The excellent activity and stability of the Cu31S16/ZnCdS are attributed to the formation of a strong internal electric field (IEF) and the Z-scheme pathway. The comprehensive experiments and theoretical calculations provide the direct evidences of the Z-scheme route. This work may offer a way for the design and development of efficient photocatalysts to achieve solar-to-chemical energy conversion at a practically useful level.

Achieving the complete mineralization of persistent pollutants in wastewater is still a big challenge. Here, we propose an efficient photo-self-Fenton reaction for the degradation of different pollutants using the high-density (Ag: 22 wt %) of atomically dispersed AgCo dual sites embedded in graphic carbon nitride (AgCo−CN). Comprehensive experimental measurements and density functional theory (DFT) calculations demonstrate that the Ag and Co dual sites in AgCo−CN play a critical role in accelerating the photoinduced charge separation and forming the self-Fenton redox centers, respectively. The bimetallic AgCo−CN exhibited excellent photocatalytic performance toward the phenol even under extreme conditions due to an efficient degradation pathway and in situ generation of the hydrogen peroxide producing the main active oxygen species (⋅OH and 1 O 2 ) and showed long-term activity in a self-design photo-Filter reactor for the purification of the phenol. Our discoveries pave the way for the design of efficient single-atoms photocatalysts-based photo-self-Fenton reaction for recalcitrant pollutant treatment.

Efficient photoinduced charge separation achieving an extremely long lifetime for improving the photocatalytic activity in hydrogen evolution reaction (HER) is essential to obtain high performance. Here, we crafted and designed the gemstone nanoflower-shaped ZnIn2S4/CuS (ZIS/CuS) heterostructure by the n-type ZIS nanoparticles grown on p-type CuS nanoflowers. The ZIS/CuS exhibited the photocatalytic HER rate of 1659 mu mol center dot g(-1)center dot h(-1) under visible light irradiation which was higher than that of ZIS nanoflower and CuS gemstone-shape. It has been attributed to the formation of type-II-scheme p-n heterojunction structure with a strong interfacial build-in electric field and the efficient photoinduced charge separation up to an ultralong lifetime of 4.89 ms. It was directly demonstrated by the in-situ X-ray photoelectron spectroscopy and femtosecond-million second transient absorption spectra (fs-ms TAS). This study provides a new strategy for constructing type-II p-n heterostructures with high photocatalytic activity and strong stability for photocatalytic HER.

There are only limited methods available to synthesize metastable olivine NaMnPO4, and these methods all involve a time-consuming process. Herein, we report a rapid synthesis of olivine NaMnPO4, and the results show that the formation of olivine NaMnPO4 highly depends on the Na/Mn/P ratio and the pH of the reaction system, and pure olivine NaMnPO4 can be hydrothermally synthesized for only 1 h under appropriate conditions. This communication provides an efficient process for synthesis of olivine NaMnPO4.

Achieving efficient spatial photoinduced charge separation and light utilization for improving the high photocatalytic activity is still a major obstacle. Here, a Cu2-xS@ZnxCd1-xS (Cu2-xS@ZnCdS) heterojunction is reported featuring a distinctive core-shell hollow nanobox structure. The Cu2-xS@ZnxCd1-xS exhibits high photocatalytic activity in hydrogen evolution reaction (HER) at the rate of 8175 mu mol center dot g(-1)center dot h(-1) under visible light irradiation, outperforming pristine ZnCdS nanoparticles and Cu2-xS hollow nanoboxes. The remarkable activity and outstanding stability of Cu2-x@ZnCdS are attributed to the development of robust interfacial electric fields, and improved light multireflection absorption efficiency as well as the Z-scheme mechanism. The electron paramagnetic resonance (EPR) and in situ X-ray photoelectron spectroscopy (XPS) measurements gave the direct evidence of the formation of the Z-scheme, which maintained the high redox potentials of each ZnCdS and Cu2-xS. This study gives the guideline for the design of heterojunction with the Z-scheme mechanism, leading to the high photocatalytic performance and remarkable stability.

Achieving high effective degradation of organic pollutants in sewage having adverse effects on human health and ecosystems remains a major challenge. In this study, an oxygen vacancy (Ov)-mediated Z-scheme Co3O4/Ov-TiO2 heterojunction was first reported for simultaneous selective photoelectrocatalytic pollutant degradation and hydrogen production under visible light irradiation. The optimized Co3O4/Ov-TiO2 exhibited excellent photoelectrocatalytic performance in the degradation of the organic pollutants under visible light irradiation due to the formation of a Z-scheme heterojunction for the utilization of highly reductive photogenerated electrons and oxidative holes. The mechanistic investigation suggested that the synergistic effects of hydroxyl radical and singlet oxygen as the dominant reactive species facilitated the ring-open reactions of the rhodamine B for the mineralization processes. This work provides a deep understanding of designing Z-scheme heterojunction photoelectrocatalysts through defect engineering technologies for sewage treatment.

Rechargeable magnesium batteries (RMBs) are cost-effective and dendrite-free, making them desirable for largescale applications. Nevertheless, the exploration of high-performance cathodes still remains a great challenge in magnesium battery research. Herein, the CoSe porous polyhedra induced by Te heteroatoms (CoSe/Te) are successfully prepared by two-step metal-organic framework (MOF)-template assisted method and investigated as high-efficiency cathodes for rechargeable MIBs. In this regard, the affluent porous structure can facilitate the transport of Mg2+ ions while the introduction of Te heteroatoms can reduce the conversion reaction barrier, boost the kinetics and redox reversibility and excite the electron conduction to build active nanostructured domains for highly reversible Mg storage reactions. As a consequence, the CoSe/Te maintains the high specific capacity of 150.6 mAh g-1 after 600 cycles at 200 mA g-1, with a superior capacity retention rate of 75.3%. Moreover, the specific capacity of such electrode materials changed from 260 mAh g-1 to 41 mAh g-1 when the current density increased from 100 mA g-1 to 2000 mA g-1, and gradually recovered to 256.5 mAh g-1 when the current density returned to 100 mAh g-1, exhibiting a better rate performance. This work highlights how micronanostructures can favor magnesium storage reaction reversibility and cyclability and also provide insights into rational electrode design for storing magnesium cations in future studies.

The effect of alkali ions (Na+ and K+) on the hydrothermal synthesis of olivine lithium metal phosphates in the P excess system was investigated by taking the synthesis of LiMn0.8Fe0.19Mg0.01PO4 as a case study. It is found that the coexisting Na+ can compete with Li+ to partly form NaMnPO4 as an impurity when the Na+/Li+ ratio exceeds the critical value, and this is not the case for the coexisting K+. These behaviors should be related to the difference in the ionic size of the alkali ions which also leads to a very different process of LiMn0.8Fe0.19Mg0.01PO4 formation. The samples derived from the K+-coexisting reaction system can deliver much higher reversible capacities as compared with the sample derived from the Na+-coexisting reaction system. This study provides new insights into the chemistry of the hydrothermal synthesis of olivine lithium metal phosphates, with an important implication for controllable synthesis and property manipulation.

The design of highly efficient and stable electrocatalysts in hydrogen evolution reaction over a wide range of pH, especially in neutral or alkaline conditions, is of great significance but remains· challenging. Herein, a family of single‐atoms and clusters inside the N‐doped porous carbon matrix (NDPCM) are encapsulated. Specifically, the single‐atom platinum (Pt SA ) and cluster platinum (Pt C ) in NDPCM exhibited ultralow overpotentials of 20 and 14 mV at −10 mA cm −2 under neutral and alkaline conditions, respectively and superior long‐term durability. Theoretical calculations and operando Raman measurements revealed that the coexistence of Pt SA and Pt C can provide multiple H adsorption sites, contributing to the extremely low |Δ G H* | of H adsorption and constructing a local acidic microenvironment to trigger a unique H 3 O + ‐induced water reduction in neutral and alkaline conditions This unique configuration significantly promotes the catalytic activity and opens a new avenue for the crafted design of electrocatalysts.

Background Artificial synaptic behaviors are necessary to investigate and implement since they are considered to be a new computing mechanism for the analysis of complex brain information. However, flexible and transparent artificial synapse devices based on thin-film transistors (TFTs) still need further research. Purpose To study the application of flexible and transparent thin-film transistors with nanometer thickness on artificial synapses. Materials and Methods Here, we report the design and fabrication of flexible and transparent artificial synapse devices based on TFTs with polyethylene terephthalate (PET) as the flexible substrate, indium tin oxide (ITO) as the gate and a polyvinyl alcohol (PVA) grid insulating layer as the gate insulation layer at room temperature. Results The charge and discharge of the carriers in the flexible and transparent thin-film transistors with nanometer thickness can be used for artificial synaptic behavior. Conclusion In summary, flexible and transparent thin-film transistors with nanometer thickness can be used as pressure and temperature sensors. Besides, inherent charge transfer characteristics of indium gallium zinc oxide semiconductors have been employed to study the biological synapse-like behaviors, including synaptic plasticity, excitatory postsynaptic current (EPSC), paired-pulse facilitation (PPF), and long-term memory (LTM). More precisely, the spike rate plasticity (SRDP), one representative synaptic plasticity, has been demonstrated. Such TFTs are interesting for building future neuromorphic systems and provide a possibility to act as fundamental blocks for neuromorphic system applications.