Jianwei Lu

Poly(vinylidene fluoride‐co‐hexafluoropropylene) (PVDF‐HFP)‐based polymer electrolytes offer a combination of flexibility, mechanical robustness, and room‐temperature ion transport for lithium metal batteries. However, residual N,N‐dimethylformamide (DMF) from electrolyte fabrication readily coordinates with Li ⁺ , forming a solvent‐dominated local environment that impedes Li ⁺ migration, increases the interfacial desolvation barrier, and slows charge–transfer kinetics. Herein, we reconstruct the residual‐solvent‐involved Li ⁺ coordination environment in PVDF‐HFP polymer electrolytes by introducing 2,2,2‐trifluoroethanamide (T3AM) as a weakly coordinating molecular regulator. The electron‐withdrawing −CF ₃ group weakens the Li ⁺ ‐binding affinity of T3AM, attenuating DMF‐dominated coordination and promoting TFSI ⁻ participation into the Li ⁺ coordination shell. The resulting anion‐rich Li ⁺ coordination structure facilitates both ion transport and interfacial desolvation. Consequently, the T3AM‐regulated PVDF‐HFP electrolyte delivers an ionic conductivity of 0.34 mS cm ⁻¹ , a Li ⁺ transference number of 0.55, and a critical current density of 3.4 mA cm ⁻² . Moreover, the regulated interfacial chemistry promotes the formation of a uniform inorganic‐rich solid electrolyte interphase, enabling stable Li||Li symmetric‐cell cycling for 1500 h and Li||NCM811 full cell with 80% capacity retention after 340 cycles at 60°C and 1C. This work highlights residual‐solvent‐involved coordination reconstruction as an effective molecular strategy for simultaneously enhancing ion transport, interfacial kinetics, and lithium‐metal stability in PVDF‐HFP polymer electrolytes.

Aqueous zinc batteries hold great promise for large‐scale energy storage due to their high energy density, safety, and cost‐effectiveness. However, the intrinsic thermodynamic instability of zinc drives inevitable HER, leading to interfacial accumulation of OH ⁻ that significantly exacerbates dendrite growth and “dead zinc” formation. This work leverages the specific structural and reactive properties of histidine (HIS) to construct a Zn(OH) ₂ ‐HIS ultrathin solid electrolyte interphase (SEI) on the zinc anode. This SEI stabilizes the interfacial pH via a synergistic mechanism of chemical buffering and physical blocking. Chemically, the imidazole and amino groups buffer the pH via reversible protonation/deprotonation; physically, the SEI disrupts the interfacial hydrogen‐bond network and repels solvated water, thereby suppressing H ₂ O‐induced side reactions. Additionally, the SEI modulates interfacial surface energy to enable (002)‐oriented deposition. Consequently, the HIS@Zn anode achieves significantly improved reversibility with a high Coulombic efficiency of 99%. It exhibits ultra‐stable cycling for over 1350 h at 10 mA cm ⁻² and 5 mAh cm ⁻² . Even at a high depth of discharge of 81%, stable operation is maintained for over 300 h. Furthermore, the HIS@Zn||MnO ₂ full cell delivers an initial capacity of 146.6 mAh g ⁻¹ at 1 A g ⁻¹ , retaining 92.33% of its capacity after 700 cycles.

In aqueous zinc‑ion batteries (AZIBs), uncontrolled dendrite growth and parasitic corrosion reactions critically limit long‑term stability. Constructing a robust organic–inorganic solid electrolyte interphase (SEI) has emerged as an effective strategy; however, the mechanistic origin of Zn‐anode stabilization remains insufficiently understood. Here, we in situ construct an ultrathin organic–inorganic hybrid SEI (Zn‐S‐RCOOH) on Zn using a multifunctional organic acid, mercaptosuccinic acid (MSA). The COOH‑rich organic outer layer restructures the interfacial hydrogen‑bond (HB) network, lowers H ₂ O activity, and accelerates desolvation, whereas the inner ZnS layer provides fast Zn ²⁺ migration pathways, collectively enhancing reaction kinetics and promoting (002) oriented Zn deposition. Owing to these synergistic effects, dendrite formation and corrosion are effectively inhibited. The MSA/Zn electrode operates stably for over 2400 h at 10 mA cm ⁻² and 5 mAh cm ⁻² , and maintains>500 h stability even at a high depth of discharge (DOD, 81 %). Moreover, MSA/Zn||MnO ₂ full cells exhibited capacities of ∼189.7 and 142 mAh g ⁻¹ with high‐capacity retention (99.18 % and 97.55 %) at 0.3 and 1 A g ⁻¹ , respectively. So, our findings proposed a rational interfacial‐engineering strategy for designing durable Zn metal anodes and advancing high‐performance aqueous zinc‐ion batteries.

Rechargeable zinc–air batteries (ZABs) are promising candidates for sustainable energy storage; however, their performance is severely limited by sluggish oxygen reduction and evolution (ORR/OER) kinetics. Here, a hard‐templating etching strategy was employed to construct nitrogen‐doped hollow mesoporous carbon spheres embedded with NiCo nanoparticles (NiCo@N‐HMCS). The hollow nanostructure, together with a strong electronic coupling between NiCo alloys and N‐doped carbon, provides abundant accessible active sites, optimized charge transfer, and robust structural stability. As a result, NiCo@N‐HMCS delivers remarkable bifunctional electrocatalytic activity in alkaline media, with a half‐wave potential of 0.84 V for the oxygen reduction reaction and an overpotential of 330 mV at 10 mA cm ⁻² for the oxygen evolution reaction. When applied in ZABs, the catalyst delivers a high open‐circuit voltage of 1.56 V, a peak power density of 185.53 mW cm ⁻² , and durable cycling over 300 h. The flexible ZAB configuration also delivers a power density of 79.06 mW cm ⁻² and stable operation of 120 h. This study demonstrates a robust platinum‐group‐metal‐free strategy for advancing next‐generation rechargeable and flexible energy storage systems.

In this work, we developed a novel method to synthesize Au nanoparticles (NPs) and a TiO ₂ nanocomposite catalyst with Au NPs embedded individually within the inner surface of a TiO ₂ bowl‐like nanostructure (nanobowl) for the first time (denoted as Au@@TiO ₂ ). This unique TiO ₂ nanobowl shell can serve as a stable support for inner Au centers, and the resulting Au@@TiO2 shows markedly improved catalytic activity in the visible‐light degradation of methylene blue (MB) compared with Au‐embedded TiO ₂ Hollow Spheres (HSs) and Au‐deposited commercial P25 (denoted as Au@TiO ₂ and Au‐P25, respectively). Our well‐established nanobowl provides a new strategy and pathway for the synthesis of high‐performance nanocomposite catalysts.

Silver nanoparticles (Ag NPs) were homogeneously deposited on the surface of silicon dioxide (SiO ₂ ) and then encapsulated by an outer titanium oxide (TiO ₂ ) layer. This SiO ₂ /Ag/TiO ₂ geometry (denoted as SiO ₂ ‐Ag@TiO ₂ nanoreactor, where “@” denotes a gap) composite was successfully developed via a conventional sacrificial method followed by partial etching. This special SiO ₂ , Ag, TiO ₂ bearing‐construction (BC) catalyst exhibits superior catalytic and exceptional stability performance when used in the degradation of methylene blue (MB) under ultraviolet light (UV light) and visible light, compared with pure TiO ₂ shell and traditional Ag/TiO ₂ yolk–shell (Ag‐TiO ₂ ). This enhanced catalytic efficiency is primarily attributed to synergistic effects derived from Ag NPs “locking and guarding” mechanism in the presence of amino‐SiO ₂ and outer TiO ₂ . In this regard, our rational BC design concept proposed a state‐of‐the‐art strategy and provided an opportunity to shorten the distance between theory and practical applications in solar conversion, such as water splitting technology, photovoltaic, and solar cells.

Slow oxygen reduction and oxygen evolution reactions (ORR/OER) kinetics of rechargeable zinc air batteries (ZABs) severely constrain the practical deployment of ZABs. Here, a novel bifunctional catalyst, nanogold‐modified NiFe‐layered double hydroxides/Co nanocluster carbon nanoframes (Au‐NiFe‐LDH/Co‐NC), is reported. This catalyst achieves a half‐wave potential of 0.826 V and a Tafel slope of 79.1 mV dec ⁻¹ , alongside outstanding OER activity, featuring a low overpotential of 300 mV at 10 mA cm ⁻² and a Tafel slope of 84.95 mV dec ⁻¹ . Notably, its Δ E value (0.704 V) is lower than that of commercial catalysts (0.746 V), validating exceptional bifunctional activity. When integrated into ZABs, this catalyst delivers a peak power density of 169.0 mW cm ⁻² , a specific capacity of 739.7 mAh g ⁻¹ , and maintains robust cycling stability over 400 cycles with minimal charge/discharge voltage polarization. Electrochemical analysis, XPS analysis, and calculations demonstrate that Au nanoclusters modulate the electronic structure of Co and NiFe‐LDH, enhancing ORR/OER activity by optimizing their d‐band structures and reducing reaction overpotentials. This work offering significant potential for applications not only to ZABs but also to other catalytic reactions.

Uniform deposition is a promising strategy to inhibit dendrite growth and corrosion of the Zn anode in cost‐effective energy storage systems: aqueous Zn‐ion batteries (AZIBs). Herein, we report a regulating Zn²⁺ ions dissolution/deposition method for achieving a highly reversible Zn anode. 11‐mercaptoundecanoic acid (MUA) as ligands was utilized to protect the (002) plane, benefiting from the strong affinity between the thiol group and Zn, with MUA anchoring in the form of Zn‐S‐RCOOH, which contributes to a stable interface for uniform deposition/deposition. More importantly, the MUA bonds to the (002) plane tightly and acts as a “rivet,” strengthening the Zn–Zn bonds of the (002) plane and leading to the high exposure of the (002) plane during the plating and stripping process. The MUA@Zn anode with 50 μm ultrathin thickness exhibits excellent stability (over 4000 h) and low overpotential at high current density (0.1–23 mA cm⁻²) and capacity (0.1–23 mAh cm⁻²). In addition, it also delivers a capacity of 194.1 mAh g⁻¹ at 1 A g⁻¹ and capacity retention of 95% after 1000 cycles. Consequently, our work provides a facial yet interfacial engineering approach in realizing the enhancement of Zn anode stability, exhibiting significant potential for practical application in AZIBs.

Bacterial cellulose (BC) as a natural polymer possessing ultrafine nanofibrous network and high crystallinity, leading to its remarkable tensile strength, moisture retention and natural degradability. In this study, we revealed that this BC membrane has excellent affinity to organic electrolyte, high ionic conductivity and inherent ion selectivity as well. Due to its ability of migrating lithium ions and suppressing the shuttling of anions across the membranes, it is deemed as available model for iodide‐assisted lithium‐oxygen batteries (LOBs). The cycle life of the LOBs significantly extends from 74 rounds to 341 rounds at 1.0 A g⁻¹ with a fixed capacity of 1000 mAh g⁻¹, when replacing glass fiber (GF) by BC membrane. More importantly, the rate performance improves significantly from 42 to 36 cycles to 215 and 116 cycles after equipping with the BC membrane at 3.0 and 5.0 A g⁻¹. Surprisingly, the full discharge capacity dramatically enhanced by ca. eight times from 4,163 mAh g⁻¹ (GF) to 32,310 mAh g⁻¹ (BC). Benefited from the convenient biosynthesis, cost‐effectiveness and high chemical‐thermal stability, these qualities of the BC membrane accelerate the development and make it more viable for application in advancing next‐generation environmentally friendly LOBs technology with high energy density.