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KAP1 with porous surface structure and reasonable hydrogen bonding are used as fillers in PEO-based CPEs that could solve the compatibility of fillers in polymer-based electrolytes and provide a valuable reference for the design of high-performance ASSLMBs. [Display omitted] Achieving practical applications of PEO-based composite solid electrolyte (CPE) batteries requires the precise design of filler structures at the molecular level to form stable composite interfacial phases, which in turn improve the conductivity of Li+ and inhibit the nucleation growth of lithium dendrites. Some functional fillers suffer from severe agglomeration due to poor compatibility with the polymer base or grain boundary migration, resulting in limited improvement in cell performance. In this paper, ILs@KAP1 is reported as a filler to enhance the performance of PEO-based batteries. Thereinto, the hypercrosslinked phosphorus ligand polymer-containing KAP1, designed at the molecular level, has an abundant porous structure, hydrogen bonding network, and a rigid skeleton structure of benzene rings. These can be used both to improve the flammability with PEO-based and to reduce the crystallinity of the polymer electrolyte. Ionic liquids (ILs) are encapsulated in the nanochannels of KAP1, and thus a 3D Li+ conducting framework could be formed. In this case, it could not only facilitate the wettability of the contact interface with the electrode, significantly promoting its compatibility and providing a fast Li+ transport path, but also facilitate the formation of LiF, Li 3 N and Li 2 O rich SEI components, further fostering the uniform deposition/exfoliation of lithium. The LFP||CPE||Li battery assembled with ILs@KAP1-PEO-CPE has a high initial discharge specific capacity about 156 mAh/g at 1C and a remaining capacity about 121.8 mAh/g after 300 cycles (capacity retention of 78.07%). [ABSTRACT FROM AUTHOR]

Total internal reflection microscopy (TIRM) measures the interactions between a colloidal particle and a flat surface in aqueous solution. Recently, TIRM has further integrated with video microscopy (VM) and enabled the simultaneous measurements of multi-particle colloid-surface interactions in the same ensemble. However, there still remain challenges about accurate image acquisition due to blooming. Blooming means the number of photons reaching the detector exceeds its maximum capacity, and the excess photons will either spill to adjacent pixels or not be counted, leading to an obstacle from precise determination of intensity. Our result shows that blooming gives rise to a deviation of the measured potential energy from the classical theory of Derjaguin, Landau, Verway, and Overbeek (DLVO). Therefore, a correction method was developed in this work to deduce the real intensity from the experimental measurement. The relationship between scattered light intensity and exposure time deviates from linearity when blooming occurs. A correction equation was developed to recover the real intensity, which was then confirmed by the accordance between the corresponding potential energy profiles and the DLVO theory. This correction method is suitable for VM systems of colloidal probes illuminated by scattered light, broadening the application of VM imaging to investigate colloidal interactions. [ABSTRACT FROM AUTHOR]

Highlights: The introduction of PEG 400 additive in the aqueous electrolyte enables regulating the Zn2+ solvation structure and inhibiting the ionization of free water molecules. Such anti-proton electrolyte can not only reduce the lattice expansion of cathode hosts and inhibit the associated by-products, but also guide the uniform Zn deposition and inhibit the hydrogen evolution reaction. A high-rate Zn-V2O3/C battery with 18,000-cycle shelf-life can be demonstrated via the integrated synergetic modification mechanism.Large volumetric expansion of cathode hosts and sluggish transport kinetics in the cathode–electrolyte interface, as well as dendrite growth and hydrogen evolution at Zn anode side are considered as the system problems that cause the electrochemical failure of aqueous Zn-vanadium oxide battery. In this work, a multifunctional anti-proton electrolyte was proposed to synchronously solve all those issues. Theoretical and experimental studies confirm that PEG 400 additive can regulate the Zn2+ solvation structure and inhibit the ionization of free water molecules of the electrolyte. Then, smaller lattice expansion of vanadium oxide hosts and less associated by-product formation can be realized by using such electrolyte. Besides, such electrolyte is also beneficial to guide the uniform Zn deposition and suppress the side reaction of hydrogen evolution. Owing to the integrated synergetic modification, a high-rate and ultrastable aqueous Zn-V2O3/C battery can be constructed, which can remain a specific capacity of 222.8 mAh g−1 after 6000 cycles at 5 A g−1, and 121.8 mAh g−1 even after 18,000 cycles at 20 A g−1, respectively. Such “all-in-one” solution based on the electrolyte design provides a new strategy for developing high-performance aqueous Zn-ion battery. [ABSTRACT FROM AUTHOR]

The preparation of Hydrogen peroxide (H 2 O 2) by electrochemical two-electron oxygen reduction reaction (2e- ORR) and water oxidation reaction (2e- WOR) is a highly desirable method that can be green, clean and safe. However, the sluggish reaction kinetics and poor 2e- ORR and WOR selectivity severely limits scale-up applications. To resolve these challenges, research on cost-effective catalysts have been intensively explored, which have made great progress. Herein, we first introduced the fundamental chemistry and catalytic mechanism of ORR and WOR, including the possible reaction pathways, the binding modes of oxygen and water on the catalytic sites, and the energy-barrier diagrams of each stage of the reaction obtained by theoretical calculations. Then, the current progress of catalyst research for electrocatalytic synthesis of H 2 O 2 is discussed. Among them, single-atom catalysts as well as molecular catalysts are the hot spots of current research. Single-atom catalysts can reduce the amount of precious or non-precious metals used, and maintain catalytic activity while reducing costs; meanwhile, molecular catalysts have the advantages of single reaction performance, high selectivity, and clear mechanism, which are easy to design and grasp. Finally, on the basis of previous studies, the remaining challenges and development prospects of the current research on electrocatalytic production of H 2 O 2 are discussed, and suggestions are provided for the development of this field in the future. [Display omitted] • The current progress of catalyst research for electrocatalytic synthesis of H 2 O 2 is discussed. • In this review, we introduced some strategies to improve the performance of H 2 O 2. • The remaining challenges and development prospects of the current research on electrocatalytic production of H 2 O 2 are discussed. [ABSTRACT FROM AUTHOR]

Most near‐infrared (NIR) light‐responsive photocatalysts inevitably suffer from low charge separation due to the elevated Coulomb interaction between electrons and holes. Here, an n‐type doping strategy of alkaline earth metal ions is proposed in crystalline K+ implanted polymeric carbon nitride (KCN) for visible and NIR photoactivity. The n‐type doping significantly increases the electron densities and activates the n→π* electron transitions, producing NIR light absorption. In addition, the more localized valence band (VB) and the regulation of carrier effective mass and band decomposed charge density, as well as the improved conductivity by 1–2 orders of magnitude facilitate the charge transfer and separation. The proposed n‐type doping strategy improves the carrier mobility and conductivity, activates the n→π* electron transitions for NIR light absorption, and breaks the limitation of poor charge separation caused by the elevated Coulomb interaction. [ABSTRACT FROM AUTHOR]

[Display omitted] Magnesium rechargeable batteries are promising candidates for large-scale energy storage due to their -high safety, low material cost, and earthabundant materials. Many redox-active polymers have recently been reported to show excellent cycling stability with decent Mg-storage performance. However, compared to their Li counterparts, these polymers exhibit lower Mg-storage capacity, resulting in a low ratio of materials utilization (η Mg/ η Li) for the same polymer in two electrolyte systems (i.e., Mg vs. Li electrolytes). Herein, we present a sulfur-linked porous polymer, poly(hexaazatrinaphthalene sulfide) (PSHATN), which sets a record for material utilization of 98% among all polymer electrodes and delivers a reversible capacity of 196 mAh g−1 in Mg electrolytes. Based on electrochemical impedance spectroscopy and operando optical microscopy, we discover a strong correlation between specific capacity and degree of electrochemical swelling of polymers in both electrolytes. Importantly, the high ratio (η Mg/ η Li) of PSHATN is ascribed to sufficient electrochemical swelling due to its large pore volume and flexible polymer nature, in contrast to linear polymers and rigid covalent organic frameworks that swell less effectively. This work highlights the critical need for polymer swelling in promoting ion transport in redox polymers for high material utilization and offers important polymer structural design insights for multivalent ion-based energy storage. [ABSTRACT FROM AUTHOR]

Deeply understanding of the chemical adsorption and polysulfide conversion reaction roles of Zinc protoporphyrin framework-embedded triple-layer nanofiber separator in Li-S batteries. [Display omitted] The practical application of Lithium-sulfur (Li-S) batteries is significantly inhibited by (i) the notable 'shuttle effect' of lithium polysulfides (LiPS), (ii) the corrosion of the lithium interface, and (iii) the sluggish redox reaction kinetics. The functional separator in the Li-S battery has the potential to provide the perfect solution to these problems. Herein a triple-layer multifunctional PVDF-based nanofiber separator, which contains GoTiN/PVDF layer on the top and bottom and ZnTPP/PVDF layer on the middle, is designed. The polarity and porous structure of this multifunctional separator can greatly improve the wettability of electrolytes and enhance the transportation of Li+. With the zinc-based porphyrin framework (ZnTPP) structure, this separator has a strong chemisorption and LiPS conversion ability, which greatly prevent the 'shuttle effect'. Consequently, the designed multilayer separator showed excellent electrochemical performance. As a result, the cell with GoTiN@ZnTPP@GoTiN nanofiber membrane displayed an initial discharge capacity of 1180 mAh/g with a benign capacity retention of 65.9% at 0.5C and high coulombic efficiency of more than 98.5% after 100 cycles. Even at 2C, it can still release a capacity of 798 mAh/g. Moreover, the remarkable capacity of 591 mAh/g could be achieved with a high sulfur load of 5.76 mg/cm2 under a current density of 0.1C. Based on these merits, this novel and scalable multifunctional separator is a promising candidate to replace the conventional PP separator for advanced Li-S batteries to deal with various challenges. [ABSTRACT FROM AUTHOR]

Abstract: In recent years, modifying cathode materials' surfaces become a popular pursuit. This paper reveals a novel spinel LiMn2O4 in situ coated with graphene-like membrane prepared using liquid-polyacrylonitrile (LPAN) as the carbon source. The structure and electrochemical performance of graphene-like membrane-coated spinel LiMn2O4 are investigated systematically. The membrane has a typical graphene-like layer carbon structure that can be applied the LiMn2O4 particles' surfaces in situ without affecting their crystal structure. Moreover, the graphene-like membrane helps to increase the particle size. The electrochemical performance reveals that coating the graphene-like membrane in situ significantly improves the discharge capacity and cycling stability of the spinel LiMn2O4. In particular, the spinel LiMn2O4 coated with a calcined 20 wt% LPAN graphene-like membrane in situ reached 131.1 mAh g−1 at room temperature, and up to 96% capacity is retained after 50 cycles at 0.1 C. The cyclic voltammetry and electrochemical impedance spectra analyses indicate that the graphene-like membrane does not influence the insertion or desertion of Li+. The improved electrochemical performance is attributed to the decreased manganese dissolution in the electrolyte and the smaller charge transfer resistance generated by the graphene-like membrane coating. [Copyright &y& Elsevier]

The role of defects in photocatalysis is rarely investigated more intuitively from the perspective of defect ionization energy (DIE), although it is the most important parameter for evaluating the depth of defect traps. Here, the crystalline poly(heptazine imide) (PHI) is adopted as an illustrative example to optimize the DIE and charge separation by regulating the carbon doping contents, ultimately activating the near-infrared photocatalytic activity. Shallow defect traps induced by doping (DIE < 25 meV) facilitate charge separation by releasing shallowly trapped carriers. In contrast, deep defect traps (DIE > 25 meV) act as non-radiative recombination centers, causing carrier quenching. More importantly, the non-radiative recombination rate in PHI is 1–2 orders of magnitude faster than the radiative recombination rate, so suppressing non-radiative recombination is more important for improving charge separation efficiency. Our work elucidates the role of defects in photocatalysis more intuitively from the perspective of DIE, and establishes a discernible relationship between DIE and photocatalytic activity. [Display omitted] • A carbon doping strategy with one stone and two birds has been proposed. • Elucidating the role of defects in photocatalysis more intuitively from the perspective of DIE. • High NIR photocatalytic activity. [ABSTRACT FROM AUTHOR]

Metal/metal-oxide heterointerfaces receive extensive attention in electrocatalysis on account of the strong synergy between the two components at the interface. However, the key factor governing such interfacial synergy is still unclear, making it extremely challenging to rationally design electrocatalyst with desired heterointerfaces. Here, we select metallic copper/cobalt-oxide (i.e., Cu/Co 3 O 4) heterointerfaces as model catalysts for the nitrate reduction reaction (NO 3 -RR) and tuned work function difference (ΔΦ) between Cu/Co 3 O 4 by introducing oxygen vacancies (O v) on Co 3 O 4. By combing experimental and theoretic results, we observe that the ΔΦ is a key factor that governs the interfacial synergy, which included the transfer of electrons from Cu to Co 3 O 4 and the spillover of hydrogen from Co 3 O 4 to Cu. Consequently, the Cu/Co 3 O 4 interface with an optimized ΔΦ displayed the best NO 3 −RR performance, outperforming most of other reported electrocatalysts. The above findings will create new opportunities for rationally designing heterointerfaces for efficient electrocatalysis by tuning ΔΦ. [Display omitted] • Tuning ΔΦ between Cu/CoO x by introducing different concentration of O v on CoO x. • The ΔΦ between Cu/CoO x plays a crucial role in controlling *H overflow and interfacial charge transfer. • A suitable ΔΦ between the Cu/CoO x is a key factor that improves NO 3 −RR electrocatalytic activity. • Optimized Cu/CoO x shows a maximum NH 3 FE of 95.1% along with a high current density to 400 mA cm−2. [ABSTRACT FROM AUTHOR]

The microrheology of thermoresponsive poly(N -isopropylacrylamide) (PNIPAM) microgel dispersions near a substrate surface is investigated using active microrheometry by incorporation of multipole magnetic tweezers with a total internal reflection microscope (TIRM). The microrheological behaviors and structural inhomogeneity of such a soft colloidal system in a near-wall case are analyzed by scaling theories with respect to the effective volume fraction of PNIPAM microgels (ϕ eff). [Display omitted] • Near-surface microrheology of PNIPAM microgel dispersions has been revealed. • G′ and G" exhibit distinct dependences on ω , T , and ϕ eff relative to bulk. • Regimes of ϕ eff with distinct scaling laws are observed in phase transitions. • Softness fluctuation can reveal the structural heterogeneity of microgel dispersions. Relative to the bulk systems, the near-wall (<500 nm) rheological responses of soft poly(N -isopropylacrylamide) (PNIPAM) microgel dispersions may exhibit distinct dependence on the frequency (ω), temperature (T), and effective volume fraction (ϕ eff) during the volume phase transitions. The microrheological behaviors are expected to be governed by the near-wall microstructure and its spatial heterogeneity. The combination of active microrheometry (multipole magnetic tweezers) and total internal reflection microscopy (TIRM) was employed to probe the structure–rheology relationships of microgel dispersions near a substrate surface. The ω , T , and ϕ eff -dependences of the storage modulus (G′), loss modulus (G"), and softness (J) were analyzed by power-law and Arrhenius-like scaling theories. The fluctuation of J was further analyzed to give a quantitative description of the inhomogeneity in the near-wall regions. (1) Remarkable differences in the rheological behaviors between the bulk and near-wall cases are revealed, where the latter shows a segmented overlap behavior in ϕ eff ; (2) Five regimes of ϕ eff that correspond to distinct physical states of the microgel dispersions are determined; (3) The near-wall local structures exhibit more heterogeneity in the glass and colloidal gel regimes as compared to the liquid regime. [ABSTRACT FROM AUTHOR]

• Constructing a series of O-doped K+ implanted CCN with narrowed bandgap (2.71-1.62 eV) for the first time. • Adopting oxygen doping strategy to activate the n→π* transition to enhance visible light and even near-infrared light harvesting. • An approximately 45- and 10- times enhancement than pristine CN and CCN for H2 generation at λ > 500 nm. • Excellent photoactive up to 650 nm owns prominent advantages over most CCN. Crystalline carbon nitride (CCN) materials with photoresponse of more than 600 nm are rare. Here, we successfully prepared a series of oxygen doped K+ implanted CCN (KCN) with narrowed bandgap (2.71−1.62 eV) for the first time. Compared with most of the O-doped amorphous CN, the optical absorption can only reach 500 nm, and a few more than 500 nm, our oxygen doping strategy is adopted to activate more n→π* transitions to enhance visible light and even near-infrared light harvesting. This active-optimized O-doped KCN accounts for 45- and 10- times promotion than pristine CN and KCN in H 2 generation under λ > 500 nm. Most importantly, its maximum active wavelength is up to 650 nm, which has obvious advantages than most CCN-based photocatalysts in the utilization of solar energy. This excellent solar capture and H 2 production is attributed to the activated n→π* electron transition, and high crystallinity and conduction band (CB) position caused by oxygen doping. [ABSTRACT FROM AUTHOR]

The role of exciton dissociation in charge separation dominated by in-plane crystallinity has been rarely addressed, although it is the decisive step of polymeric carbon nitride (CN) photocatalysis. Here, taking ten kinds of crystalline carbon nitride (CCN) as examples, the relationship between exciton dissociation, carrier mobility, conductivity, charge separation and photocatalytic activity under different in-plane crystallinity has been investigated. Although the in-plane crystallinity dominates charge separation and photocatalytic activity, it does not significantly reduce excitons binding energy (EBE) or improve exciton dissociation efficiency (EDE), only decreasing by 1.5 meV and increasing by 2.3 %, respectively. It is the greatly improved carrier mobility and conductivity that are more responsible for the increased charge separation and photocatalytic activity than the slight change in EDE. To our knowledge, this is the first reported case of overall water splitting in CCN of poly(heptazine imide) structure, resulting from the optimized in-plane crystallinity. [Display omitted] • Demonstrating the role of exciton dissociation in charge separation dominated by in-plane crystallinity. • Providing modification strategies for layered photoelectric conversion materials. • The first reported case of overall water splitting in CCN of poly(heptazine imide) structure. [ABSTRACT FROM AUTHOR]

• The Fe-doped cathode exhibited superior catalytic activity for CO 2 reduction compared to pristine La 0.5 Sr 0.5 MnO 3. • The incorporation of Fe into the unit cell increased its size and facilitated the CO 2 reduction activity. • Fe substitution improves CO 2 adsorption and decreased the energy barrier of the rate-determining step. • The Fe-doped cathode resulted in an increased maximum power density in the Zn-CO 2 battery. Aqueous Zn-CO 2 batteries are a new technology for reducing carbon dioxide emissions and converting CO 2 into valuable products. The development of high-performance catalysts is crucial for improving the efficiency of the CO 2 reduction reaction(CO 2 RR) in these batteries. The technical challenges of CO 2 RR catalysts include high cost, complicated synthesis and low Faraday efficiency. In this study, we developed an efficient and cost-effective CO 2 RR perovskite catalyst, by partially substituting Fe to the B site of precious metal-free La 0.5 Sr 0.5 MnO 3 (LSM) perovskite. Comprehensive investigation into the Structure, morphology, coordination information and electrochemical performance of pristine La 0.5 Sr 0.5 MnO 3 (LSM) and substituted La 0.5 Sr 0.5 Fe 0.6 MnO 3 (LSF 0.6 M) catalysts were conducted, LSF 0.6 M catalyst shows enhanced electrochemical performance, Faraday efficiency, battery durability and battery power density than LSM. Specifically, the Fe-doped catalyst shows a significant improvement in CO 2 reduction reaction (CO 2 RR) performance, with an 80% increase in current density, an 82% Faraday efficiency, and a 50% increase in power density of Zn-CO 2 battery. Characterization experimental results and DFT calculation reveal that Fe substitution can increase the perovskite lattice size to favor CO 2 absorption and *COOH formation, thus the improved CO yields. These analyses provided insights into the underlying mechanisms of the catalyst's performance in CO 2 RR within the battery system. These results highlight LSF 0.6 M perovskite as a very promising CO 2 RR electrocatalyst for Zn-CO 2 battery. [ABSTRACT FROM AUTHOR]

• Facile synthesis of amorphous VO 2 –crystalline NiS 2 heterostructures. • Identifying the different co-catalytic function of VO 2 for boosting the HER and OER. • VO 2 tunes the binding energy of NiS 2 with hydrogen intermediates to enhance the HER activity. • VO 2 alters the electrochemical reconstruction behavior of NiS 2 during the process of OER. • The obtained VO 2 / NiS 2 requires a low voltage of 1.53 V at10 mA cm−2 for overall water splitting. The rational design of bifunctional electrocatalysts is essential to achieve efficient hydrogen production from water splitting. Here, inspired by cocatalysts widely utilized in photocatalysis, we designed a heterostructure comprising amorphous VO 2 and crystalline NiS 2 , aiming at using VO 2 cocatalyst to boost activity of NiS 2 for both the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). Intriguingly, we found that VO 2 displayed different co-catalytic function in boosting the OER and HER. Specifically, the VO 2 optimized the binding energy of hydrogen intermediate on NiS 2 and thus improved the HER activity. As for the OER, the amorphous VO 2 was easily dissolved in the KOH electrolyte, resulting in the generation of abundant oxygen vacancies in the in-situ generated active phase of NiOOH from NiS 2 , thereby drastically enhancing the OER activity. Consequently, the obtained VO 2 –NiS 2 @CC displayed excellent performance for overall water splitting, with a low voltage of 1.53 V at 10 mA cm−2. [ABSTRACT FROM AUTHOR]

Graphical abstract Highlights • LSFT is used as anode electrocatalyst for hydrocarbon fueled SOFC. • LSFT shows good electro-activity toward CH 4 direct oxidation. • LSFT keeps stable in H 2 fuel with different H 2 S contents up to 750 ppm for 24 h. • LSFT presents a good carbon deposition tolerance. Abstract Efficient and direct utilization of hydrocarbon fuel in a solid oxide fuel cell (SOFCs) is highly desirable. However, the carbon deposition and contaminants poisoning issue should be overcome. In this work, we developed a titanium-doped (La,Sr)FeO 3 ceramic oxide (LSFT) anode which integrates the advantage of high durability of titanate perovskite and super electrocatalytic activity of ferrite-based perovskite for methane-fueled SOFCs with H 2 S impurity. Its electrocatalytic activity and operational durability in H 2 with various H 2 S contents and humidified CH 4 fuel were systematically investigated. We found that the LSFT perovskite oxide anode showed acceptable activity and durability toward methane direct oxidation, and excellent coke and sulfur tolerance up to 750 ppm, making it a promising electrocatalyst for direct use of hydrocarbon fuels such as natural gas in high-temperature SOFCs. [ABSTRACT FROM AUTHOR]

Graphical abstract Highlights • MoS ` -NiS x electrocatalysts are prepared by scalable mechanical ball milling method. • NiS x addition exposes edge sites of MoS 2 and creates active hetero-interfaces. • Synergistic effect takes place in the heterostructure MoS 2 -NiSx. • Ni-Mo-S (1:1:10) give the best HER activity (Tafel slope 66 mV dec−1 and η 10 83 mV), better than literature. Abstract Hydrogen generation by electrochemical water splitting with the renewable power source is one of the most promising pathways for green and sustainable society. The challenge is to explore a simple and cost-effective method to synthesize earth-abundant and noble-metal-free electrocatalysts with reliable hydrogen evolution reaction (HER) activity. Herein, we report a facile and scalable method to synthesize hybrid MoS 2 and nickel sulfides (NiS/NiS 2 /Ni 3 S 4) nanosheets (Mo-Ni-S NSs) with highly efficient HER activity in alkaline media. The hybrid phase and NSs allow large exposure of edge sites of MoS 2 and construct highly active hetero-interfaces between MoS 2 and NiS x and sufficient durability in alkaline solution. Mo-Ni-S NSs with optimal composition presents a low overpotential of 83 mV to reach a current density of 10 mA cm−2 in 1.0 M KOH, which is comparable to the performance of recent reported highly active MoS 2 based electrocatalysts. This work sheds light on the facile synthesis of multiple heterostructures as efficient electrocatalysts for scalable application in energy chemistry. [ABSTRACT FROM AUTHOR]

The efficient and sustainable production of high-purity hydrogen gas through electrochemical water splitting calls for robust and bifunctional catalysts to accelerate the two half reactions of water splitting. Herein, we in-situ craft ultrathin CoNi-sulfides nanosheet (∼2.2 nm in thickness) arrays-anchored MnO 2 nanoparticles (∼3.2 nm in diameter) (denoted U-CoNi-S-NSA/MnO 2 ) via a spontaneous redox process between CoNi-sulfides nanosheet and MnO 4 − anions at ambient temperature. The hierarchical U-CoNi-S-NSA/MnO 2 nanocomposites are then directly employed as self-supported catalysts for the two half reactions of water splitting, showing excellent activity with small overpotentials of 170 mV for oxygen evolution reaction and 67 mV for hydrogen evolution reaction to achieve 10 mA cm −2 , respectively. Moreover, an efficient water electrolyzer through using U-CoNi-S-NSA/MnO 2 as both anodic and cathodic catalysts is fabricated, which achieves current density of 10 mA cm -2  at a small voltage of 1.51 V over a long-time operation of 20 h. This outstanding performance is markedly superior than that of precious Pt/C//RuO 2 counterpart (1.61 V). Therefore, the as-synthesized hierarchical nanocomposites are promising candidates for cheap and efficient water splitting. [ABSTRACT FROM AUTHOR]

Highly conductive ceria-carbonate composite represents one type of most promising electrolyte materials for low temperature solid oxide fuel cells (SOFCs). Composites with large oxide-carbonate interface and homogeneous element/phase distribution are desirable to further enhance electrical properties and to study the ionic conduction mechanism. In this work, we report the successful synthesis of element/phase well-distributed, interfacial strongly coupled Sm 0.2 Ce 0.8 O 2 -Na 2 CO 3 (NSDC) nanocomposite with different residual carbonate contents by an in-situ one-pot one-step citric acid-nitrate combustion method. Interestingly, NSDC shows distinct properties over those prepared by conventional methods and improved ionic conductivity. In particular, NSDC9010 nanocomposite displays a proton conductivity of 0.044 S cm −1 at 650 °C, which is 3–5 times higher than the oxide proton conductors. Electrolyte supported SOFCs based on the resultant nanocomposite electrolyte, NSDC9010, give the best power output of 281.5 mW cm −2 at 600 °C with LiNiO 2 symmetric electro-catalysts. The excellent ionic conductivity and fuel cell performance are correlated with the unique core-shell structure, good phase distribution and large interfacial area induced by the one-step fabrication method, the strong coupling between oxide and carbonate as verified by the differential thermal and Raman spectroscopy characterization results and the optimal interfacial carbonate layer thickness by intentionally adjusting of carbonate contents. [ABSTRACT FROM AUTHOR]

Block copolymer prodrugs (BCPs) have attracted considerable attentions in clinical translation of nanomedicine owing to their self-assembly into well-defined core-shell nanoparticles for improved pharmacokinetics, stability in blood circulation without drug leakage, and optimized biodistribution. However, a cascade of physiological barriers against specific delivery of drugs into tumor cells limit the final therapeutic efficacy. Herein, we report a robust and facile strategy based on thiolactone chemistry to fabricate well-defined BCPs with sequential tumor pH-promoted cellular internalization and intracellular stimuli-responsive drug release. A series of BCPs were prepared through one-pot synthesis from clinically used small molecule anticancer drugs. The ring-opening reaction of drug-conjugated thiolactones releases mercapto groups via aminolysis by N -(3-aminopropyl)-imidazole, which further react with poly(ethylene glycol)- block -poly(pyridyldisulfide ethylmethacrylate) (PEG-PDSEMA) to produce imidazole and disulfide bonds-incorporated BCPs. Taking paclitaxel (PTX) for example, PTX BCPs exhibited high drug-loading content (>50%) and low critical micellization concentration (5 × 10 −3 g/L), which can self-assemble into micellar nanoparticles in aqueous solution with a small size (∼40 nm). The nanoparticles showed high tumor accumulation and uniform distribution in hypopermeable tumors via systemic administration. Meanwhile, imidazole moieties endow nanoparticles tumor pH-sensitive charge transition from nearly neutral to positive, which promoted cellular internalization. Disulfide bonds can be cleaved by intracellular glutathione (GSH) of cancer cells, which accelerate the release of active PTX drug inside cells. Finally, highly aggressive murine breast cancer 4T1 tumor and hypopermeable human pancreatic adenocarcinoma BxPC3 tumor were completely ablated after treatment by PTX BCP nanoparticles. Consequently, the robust and facile preparation strategy based on thiolactone chemistry represents an efficient approach to construct multifunctional BCPs for better therapeutic efficacy via addressing multiple physiological barriers. [ABSTRACT FROM AUTHOR]

Rational designing of efficient bifunctional oxygen electrocatalysts is significantly important but rather challenging for rechargeable zinc-air batteries. Herein, a novel high-performance bifunctional oxygen electrocatalyst for rechargeable zinc–air batteries are constructed based on bimetal Mn@Co-N-C encapsulated in in situ grown N,S-doped graphitic carbon framework with within a porous three-dimensional (3D) structure. The final catalyst shows a high half-wave potential of 0.89 V for oxygen reduction reaction, and a low operating overpotential of 0.38 V to achieve a 10 mA cm−2 current density for oxygen evolution reaction. The physical characterizations reveal that a strong synergetic coupling between bimetal Mn@Co-N-C and S dopant can effectively increase the active sites, meanwhile achieve a rational manipulation of the active site configuration toward a favorable electronic structure. Impressively, the assembled zinc–air batteries using liquid electrolytes and the all-solid-state batteries with this catalyst exhibit excellent charging–discharging performance, long lifetime, and high flexibility. [Display omitted] • The second metal source is Mn, which utilizes a controlled self-assembly method to orient on N, S-doped carbon-based materials generated from MOFs. • The synthesized Mn@Co-NS catalyst exhibits excellent bifunctional electrocatalytic activity. • The reasons for the superior performance of Mn@CO-NS catalysts are revealed. • Mn@Co-NS has good performance and long-term stability in the field of zinc-air batteries. • It provides direction guidance for the qualitative landing of various metals on carbon substrates, bringing the application of zinc-air batteries to a new level. [ABSTRACT FROM AUTHOR]

The built-in electric field kinetically controlled by in-situ polarization of the battery's inherent electric field and extra piezoelectric potential induced by volume expansion effectively accelerate Na+ transport, just 1 min to charge 99% at 10 A·g−1. Such outstanding tolerance and high-rate sodium storage capacity have implications for sodium-ion battery fast charging technologies. [Display omitted] • Three-dimensional core–shell BTO@SnO 2 @P-C composites are designed. • BTO@SnO 2 @P-C delivers excellent cycle tolerance and high-rate Na+ storage capacity. • The BIEF and extra piezoelectric potential effectively accelerates Na+ transport. • Confirms kinetically reversible BIEF and irreversible piezoelectric potential. Batteries with high storage capacity, durable cycle lifetime and fast charging are extremely rare but meaningful. Herein, the three-dimensional core–shell structure with tin dioxide coated barium titanate (BTO) and the outermost layer covered with phosphorus doped carbon (BTO@SnO 2 @P-C) is designed as an anode for sodium-ion batteries (SIBs), which shows remarkable cycle tolerance and high-rate sodium storage capacity. It exhibits rapid kinetics at 10 A·g−1 with a powerful life of 10,000 cycles, just 1 min to charge 99%. Such advanced electrochemical performance is primarily attributed to the built-in electric field (BIEF) generated by the in-situ dynamic polarization of BTO from the battery's inherent electric field. Additionally, ensuring the piezoelectric potential through the core–shell structure intensifies the BIEF. The BIEF effectively accelerates sodium ions transport and greatly improves tin dioxide anode reaction kinetics and sodium storage capacity, which is of constructive significance for realizing SIBs with high energy density and fast charging capability. [ABSTRACT FROM AUTHOR]

The introduction of TMP changes the coordination environment of Zn2+ to reshape the hydrogen bond network of water. A novel strategy is established to regulate Zn2+-solvation shell, restraining vanadium dissolution, suppressing Zn dendrite formation and contributing to uniform deposition of Zn2+. [Display omitted] • A novel Zn2+-solvation shell is formed via trimethyl phosphate. • Zn symmetrical battery exhibits an ultralong cyclic lifespan for 7000 h at 1 mA cm−2. • The cathode dissolution and self-discharge of battery are efficiently suppressed. • Zn|VO 2 (B) cell possesses 97.86% capacity retention after 1200 cycles at 1 A·g−1 (0 °C). The wide-scale application of zinc-ion batteries (ZIBs) is largely restricted by dendrite formation, hydrogen evolution corrosion and capacity fading, caused by the coordinated H 2 O within the Zn2+-solvation shell as well as reactive active water in the bulk electrolyte. Here, one green and flame-retardant additive, trimethyl phosphate (TMP) is introduced into aqueous electrolyte systems, contributing to Zn2+-solvation shell reshaping and promoting the stability hydrogen bonding network of H 2 O. The strategy is significant in suppressing water-induced side reactions and dendrite growth, enabling an ultralong cycling lifespan of 7000 h at 1 mA·cm−2 and 0.5 mAh·cm−2 in Zn symmetrical cell. In addition, Zn|VO 2 (B) full cells with TMP addition exhibit an ultralong cyclic performance for 1200 cycles at 1 A·g−1 with 97.86% capacity retention even at 0 °C, which contributes to taking a step closer to commercial application. This work demonstrates the feasibility of developing electrolytes for practical ZIBs that integrate safety, sustainability and wide-temperature applications. [ABSTRACT FROM AUTHOR]

[Display omitted] • Identifying that the surface-supported electrocatalysts are actually not stable under harsh condition towards the practical applications. • A lattice-confined approach is developed to concurrently enhance the stability and intrinsic activity of Ru. • Lattice-confined Ru delivers both outstanding activity and stability for HER under harsh conditions. • Both experimental and theoretical results reveal that the lattice-confined strategy significantly enhances the interaction of Ru/TiO 2. Ru-based nanomaterials are among the best electrocatalysts for hydrogen evolution reaction (HER) in alkaline media, however their stability is still questionable, especially under harsh conditions towards practical applications (i.e., 80 °C, 6 M KOH). We demonstrate that the conventionally surface-supported Ru electrocatalysts are actually not stable under harsh conditions due to the weak interaction between Ru and supports, although they are stable under mild conditions. Here, we report a lattice-confined approach to concurrently enhance the stability and intrinsic activity of Ru via confining ultrafine Ru clusters into TiO 2 lattice frameworks. Impressively, such confined Ru delivers outstanding performance for HER under harsh conditions, such as a small overpotenital of 116 mV at 800 mA cm−2, and long-time stability for 200-h continuous HER at 300 mA cm−2. As uncovered by both computational and experimental results, the lattice-confined strategy can significantly enhance the interaction between Ru and TiO 2 for promoting the electron transfer from Ru to TiO 2 , thereby strongly stabilizing Ru for avoiding the dissociation and aggregation of Ru during the stability test. Therefore, the lattice-confined strategy may stand out as a robust approach for boosting the activity and stability of electrocatalysts. [ABSTRACT FROM AUTHOR]

Single-atom catalysts (SAC) stabilized by nitrogen in carbon support are promising candidates for oxygen reduction reaction (ORR). However, conventional preparation methods usually lead to encapsulation of metallic centers in matrix and thus the utilization efficiency (UE) is underexploited. Herein, we report a novel strategy to prepare an Fe-SAC with all Fe atoms anchored on the surface of carbon nanospheres, which exhibited an extraordinary UE of 80% for ORR. This efficiency was achieved by coating polydopamine spheres with silica, followed by the pyrolysis of their blend with FeCl 3. During thermal treatment, Fe migrates across the silica shell by atomic exchange with silicon, which inhibits the aggregation of Fe and allows Fe atoms to anchor on the surface. As such, it showed excellent ORR activity at a low Fe content. Zn-air batteries assembled using this catalyst showed a peak power density of 113 mW cm−2 and specific capacity of 710 mAh g Zn −1. [Display omitted] • A single atomic Fe catalyst anchored on carbon nanosphere was prepared. • All Fe species were single-atomic and fully exposed due to restriction of silica. • The method can be extended to prepare other single-atom catalysts. • The catalyst exhibited excellent catalytic performance at a low loading of Fe. [ABSTRACT FROM AUTHOR]

The precise design and controllable manufacture of electrocatalysts for efficient oxygen reactions (OER and ORR) based on the abundant elements of the earth are urgently required but challenging task. In this study, a CoS 2 /Cu 2 S heterostructured composite (CoS 2 /Cu 2 S-NF) supported by the porous carbon nanofibers is synthesized as a high-efficiency oxygen reaction electrocatalyst. As indicated from in-situ characterization methods (infrared, Raman and XRD) integrated with the density functional theory results, the heterostructures exhibited by CoS 2 and Cu 2 S could be regulated. The results show that the electron transfer/interaction between CoS 2 and Cu 2 S in the heterojunction were regulated, as well as the electronic structures of Co and Cu sites. As impacted by the structural engineering and the electronic modulation, the activity was enhanced, and the performance of electrocatalytic oxygen reactions was improved, which exhibited the lowest potential difference for (ΔE = 0.73 V) compared with commercial electrocatalysts. The liquid ZAB in accordance with on CoS 2 /Cu 2 S-NF exhibited a stable charge and discharge capacity up to 590 h and a great power density reaching 260.60 mW cm−2. Moreover, the flexible solid-state ZAB based on CoS 2 /Cu 2 S-NF exhibited a great competitive power density (92.06 mW cm−2), robust flexibility and an obvious integration. As compared with single metal sulfide-NF, the Density functional theory calculations (DFT) highlight the adsorption on CoS 2 /Cu 2 S-NF side surface in the heterojunction, which more specifically demonstrates the synergistic effect in the junction. This work presents a direction for designing heterostructured junctions as electrocatalyst and moreover its great application potential in rechargeable metal-solid batteries. [Display omitted] • Heterostructure CoS 2 /Cu 2 S-NF shows outstanding catalysis activity for OER and ORR. • The electrocatalytic mechanism is revealed by DFT calculation and in-situ techniques. • CoS 2 /Cu 2 S-NF employing Zn-air battery displays excellent performance. • The flexible Zn-air battery was fabricated by using CoS 2 /Cu 2 S-NF. [ABSTRACT FROM AUTHOR]

[Display omitted] • A universal, facile and ultrafast precipitation polymerization method is developed. • Dual-aldehyde monomers are adopted to prepare hierarchical polymer particles. • Without using templates, hydrothermal devices, surfactants and catalysts. • The preparation process just cost 10 minutes. • Representative WBL carbon microsphere anodes exhibit high performance for LIBs. Hierarchical polymer architectures have attracted considerable attention owing to their crucial roles in catalysis, drug delivery, biology, electronics and energy storage fields. Unfortunately, the current synthesis of polymer particles with hierarchical structures mainly relies on templates, hydrothermal devices, surfactants, and catalysts approaches that have the disadvantages of time-consuming procedures, complex manufacturing processes, high cost, the use of toxic agents (e.g. HF acid for templates removal) and potential risk of explosion (hydrothermal methods). Herein, for the first time, we have developed an ultrafast template-free, hydrothermal-free, surfactant-free, and catalyst-free precipitation polymerization method to synthesize a diversity of polymer particles with multi-dimensional (0D, 1D, 2D and 3D) hierarchical structures simply from polymerization of common dual-aldehyde and amino monomers at room temperature, and the fabrication process only took 10 min. After carbonizing one typical polymer particles (wool-ball-like structure) as an application example, we further tested the electrochemical performance of the as-obtained typical structures and the results show a reversible lithium-ion storage capacity of 226.5 mAh g−1 after 3200 cycles at the current density of 5 A g−1. Our technique provides a cost-effective, rapid, scalable, and green approach to prepare multi-dimensional hierarchical polymer structures and paves the way towards their application in a diversity of emerging fields. [ABSTRACT FROM AUTHOR]

• The layered multi-anionic Ni(SO 4) 0.3 (OH) 1.4 @rGO nanocomplexes were first optimally fabricated for Li-ion battery anodes. • The optimized anode delivers greatly superior lithium storage performance. • The in-situ XRD results first reveal the multi-electro conversion mechanisms for the unique anode. • The graphene wrapping offers great electronic conductivity. The multielectron reaction materials for lithium-ion batteries are interesting charge storage hosts for next-generation high-energy–density anodes. As a class of multiple-anion transition metal compounds (MATMCs), the layered Nickel hydroxide sulfate (NiSH) nanobelts integrate positive-charged cations and intercalated anions, can be expected to construct the advanced high-energy–density materials, but have not yet reported. Herein, the layered NiSH nanobelts grafting on the 3D porous reduced Graphene oxide (rGO) nanosheets were fabricated for the first time as the negative electrode of lithium-ion battery (denoted as NiSH@rGO) by a one-pot hydrothermal approach. As expected, the NiSH@rGO composite delivers a superior initial discharge capacity (1060 mAh g−1 at 200 mA g−1 after 230 cycles) and an exceptional rate capacity (991 mA g−1 at 2000 mA g−1). Through in-situ XRD, ex-situ SEM and TEM, we showed that the outstanding performance of NiSH@rGO anode originate from multielectron reaction mechanism and prominent structural, which render expose more active sites for charge storage, increase the surface wettability of anode, accelerate electron/ion diffusion and ensure the stability of the structure. Above that, it showed excellent lithium storage capacity and high-rate performance. Furthermore, a full cell composed of the NiSH@rGO anode and LiFePO 4 cathode displays an impressive capacitance and low-capacity decay rate. Our findings fundamentally and experimentally provide insights into the multi-anionic compounds for markedly enhancing the performance of the multi-electron anodes for advanced high-capacity lithium-ion battery. [ABSTRACT FROM AUTHOR]

[Display omitted] • DFT calculation reveals the highly zincophilic properties of N,O dual-doping sites. • Zn deposition can be regulated by functionalized carbon nanofiber (CNF) interlayers. • The modified Zn anodes exhibit excellent plating/stripping reversibility. • Interfacial transport kinetics was studied by in-situ EIS technique. Although the intrinsic safety, low cost, and high theoretical energy densities have made the Aqueous zinc-ion batteries (AZIBs) to be a promising candidate in the application of energy storage fields. However, battery failure caused by the dendrite formation has become the major issue that disrupt their practical application. To solve that, herein, we report a unique interface strategy for regulating the interfacial electrodeposition kinetics and inhibiting dendrite formation through covering a N,O co-doped Carbon nanofiber (CNF) interlayers on Zn metal anode surface. Such CNF interlayers with robust zincophilicity can effectively capture the Zn ions, and guiding the regular Zn electrodeposition in the anode-electrolyte interface, which have been demonstrated by both theoretical calculation and experimental results. Significantly, the electrochemical tests confirmed that the cell modified with CNF interlayers exhibits a high Zn plating/stripping reversibility with a low nucleation overpotential. Notably, the modified cell enables steadily operating for 1200 h with a low overpotential of 59.5 mV at a high current density of 5 mA cm−2 (1 mAh cm−2). Moreover, the rate capability and cyclic stability of Zn-MnO 2 full battery can be greatly improved after covering the CNF interlayers on the Zn metal anode surface. This work is highly expected to provide a new route to enable dendrite-free Zn metal anodes and high-performance AZIBs. [ABSTRACT FROM AUTHOR]

Abstract: 1,2-Dimethyl-3-hexadecylimidazolium bromide, which lacks an acidic proton at the C-2 imidazolium ring position, exhibits thermotropic SmA2 phase behavior above its melting point of 90.3°C and up to 232.1°C. The corresponding layer spacing and the full width at half maximum from XRD patterns display a temperature dependence. In binary mixtures with water, over a concentration range of 40–75%, lyotropic liquid crystalline phases form between 0.5 and 25°C. The molecules of the new ionic liquid (IL) in the binary mixtures show three different self-assembly processes, namely, formation of rod micelles, coexistence of rod micelles and a hexagonal phase, and a pure hexagonal phase. The distance between the two centers of adjacent columns of cylinder units remains nearly constant at 4.97±0.04nm when the IL content exceeds 70%, indicating that the cylinder units attain a dense and highly ordered packing. [Copyright &y& Elsevier]

Abstract: Ternary mixtures of 1,2-dimethyl-3-hexadecylimidazolium bromide/1-decanol/water form two types of well-ordered lyotropic ionic liquid crystals, a hexagonal phase linked to the ionic liquid–water axis, and a lamellar phase located at the center of their phase diagram. The lamellar and hexagonal phases span a wide temperature range from 3 to 40°C, depending on the composition. The spontaneous self-assembly of the mixtures arises from strong association between the hydroxyl groups of 1-decanol or water and the polar head-groups of the ionic liquid (head-group solvent), aromatic stacking interaction between the imidazolium rings and the hydrophobic effect. [Copyright &y& Elsevier]

• A nature-inspired etching strategy is developed for the construction of karst topography (KT)-featured electrode. • The KT architecture offers a "superaerophobic" surface for rapidly releasing O 2 bubbles during electrocatalysis. • Experimentally identifying that the core-shell structure optimizes the adsorption strength of *OH intermediates. • The obtained electrocatalysts achieve the large current densities of 1500 mA cm−2 at an overpotential of 380 mV. Exploring of electrocatalysts for high-output oxygen evolution reaction (OER) is key to practical applications, but still remains challenging. Here, we developed a nature-inspired etching strategy for the construction of karst topography (KT)-featured electrode comprising core-shell structured Ni(0)@Ni(II) towards efficient OER. Intriguingly, the KT architecture confers a "superaerophobic" surface to render the large amount of generated O 2 bubbles release rapidly and timely from the electrode surface at the high current density of OER (i.e., 1500 mA cm−2). Moreover, this strategy allows good control over the generated core-shell structure for promoting the heterointerface synergetic effect of Ni(0)@Ni(II). By adding probing molecules to react with OER intermediates under operation conditions, we obtain first direct experimental evidence that the core-shell structure can optimize the adsorption strength of *OH for significantly boosting the OER kinetics. Notably, the obtained electrode has excellent performance for OER with a small overpotenital of 380 mV at 1500 mA cm−2. [ABSTRACT FROM AUTHOR]

A novel structure of Fe-doped NiO coupled Ni cluster hollow nanotube arrays (Fe-NiO-Ni CHNAs) composed of defect-rich NiO phase and Ni clusters anchored on outside of nanotubes is presented. The d-band downshifted by Fe-doping, coupled of Ni clusters and defect-rich nature greatly improve electrocatalytic performances of Fe-NiO-Ni CHNAs toward oxygen evolution reaction. • A multi-level structure of Fe-doped NiO coupled Ni cluster hollow nanotube arrays (Fe-NiO-Ni CHNAs) was synthesized as a catalyst for OER. • Fe-NiO-Ni CHNAs exhibits overpotential of 245 mV at 10 mA cm−2 and outstanding durability that surpasses most of transition metal oxides. • The improved OER activity is mainly because Fe doping downshifts the d-band of metal sites. • Fe-NiO-Ni CHNAs obeyed the adsorbate evolution mechanism with a nonconcerted proton-electron transfer pathway. Herein we present a novel multi-level structure of Fe-doped NiO coupled Ni cluster hollow nanotube arrays (Fe-NiO-Ni CHNAs) grown on carbon fiber cloth as an efficient catalyst for oxygen evolution reaction. In this multi-level structure, rocksalt-type Fe-doped NiO phase hybrids with Ni clusters coupled into the nanospheres anchored to the outside of nanotube, forming a unique 3D corn-like structure. This novel multi-level structure represents a large specific area for catalytic reaction. X-ray absorption fine structure indicates that the defect-rich Fe-doped NiO phase has abundant coordinative unsaturated sites as active sites, and Fe doping downshifts the d-band of metal sites, which is the main contribution to the improved oxygen evolution reaction catalytic activity. The OER of Fe-NiO-Ni CHNAs obeys the adsorbate evolution mechanism with the nonconcerted proton-electron transfer pathway as a rate-determining step. Thus Fe-doped NiO CHNAs exhibits excellent OER performance and outstanding durability that surpasses most of transition metal oxides. [ABSTRACT FROM AUTHOR]

• A material composed of MoS 3 and MXene is proposed by an electrostatic self-assembly. • MoS 3 exhibits impressive electrochemical performance in LIBs and in LSBs. • Ex-situ XPS was used to explore the electrochemical mechanism both of LIBs and LSBs. • We conceived the mechanism of LIBs and adsorption and catalytic mechanism of LSBs. The development of electrode materials with the synergistic effects of good chemical stability and high electrical conductivity has improved the sluggish ion kinetics and severe capacity degradation of rechargeable lithium batteries. Herein, a multifunctional heterostructure material (MoS 3 -Ti 3 C 2 T x) comprising a functionalized MXene (Ti 3 C 2 T x) and amorphous MoS 3 is prepared by a scalable electrostatic self-assembly method. Remarkably, as lithium-ion battery anodes, the resultant MoS 3 -Ti 3 C 2 T x not only exhibits increased electrochemical activity, accelerated lithium-ion diffusion and fast charge transfer kinetics but also shows high specific capacity, excellent rate performance and long-term cycling stability. By virtue of these merits, MoS 3 -Ti 3 C 2 T x offers an excellent reversible capacity of 1043 mAh g−1 at 200 mA g−1 and exhibited a capacity of 568 mAh g−1 at a current density of 2 A g−1 after 1000 cycles. When acting as the cathode for lithium-sulfur batteries, the amorphous MoS 3 anchored on MXene demonstrates high capture and catalytic activity towards polysulfide conversion. Accordingly, the optimized electrode exhibits a capacity of 836 mAh g−1 at 0.2C after 100 cycles and a satisfactory rate performance of 463 mAh g−1 at 2C after 400 cycles. Moreover, the associated conversion mechanism is studied by ex situ XPS. These results demonstrate that heterostructure composites constructed by an amorphous sulfide and surface functionalized MXene are feasible electrode materials for both lithium-sulfur batteries and lithium-ion batteries. [ABSTRACT FROM AUTHOR]

• High-performance heterostructure MoS 2 @SnS-QDs/CNN anode material is facile prepared. • The synergistic coupling effect among the different components is clearly revealed. • MoS 2 @SnS-QDs/CNN displays high discharge performance and excellent cycle stability. • The Li+ ions storage mechanism is investigated by in-situ XRD, ex-site XPS/SEM. • A full cell is also successfully fabricated to study the practical application. Transition metal sulfides have high abundance and large theoretical capacities are considered to be an effective candidate for advanced electrodes of lithium ion batteries (LIBs). Here, a large-scale and controllable method was used in synthesizing ultrathin MoS 2 nanosheets anchored on 3D hierarchical nanohybrids with SnS quantum dots, which are decorated on a carbon nanosheet network (MoS 2 @SnS-QDs/CNN). The 3D cross-linked carbon nanosheet not only could prevent SnS from being directly exposed to the electrolyte but also retained the structural stability of the electrode. Moreover, the MoS 2 nanosheets exposed active sites to carry lithium ions. A heterojunction was formed at the interface owing to the close contact between molybdenum disulfide and SnS and greatly increased charge carrying and lithium storage capacities. Benefiting from these structural advantages, the MoS 2 @SnS-QDs/CNN electrodes showed outstanding electrochemical and long-term cycling performance owing to their unique structures and amazing synergies. As a half-cell anode material, MoS 2 @SnS-QDs/CNN-2 provided a reversible capacity of 713 mAh g−1 after 1000 cycles at a current density of 2 A g−1. When assembled into a full battery, it still provided 491 mAh g−1 at a current density of 1 A g−1 after 100 cycles. At the same time, a small LED bulb was lit for a while. This advanced material has great potential in other applications, such as supercapacitors, catalysis, and sensors. [ABSTRACT FROM AUTHOR]