The electrocatalytic reduction of CO₂ is a promising pathway to generate renewable fuels and chemicals. However, its advancement is impeded by the absence of electrocatalysts with both high selectivity and stability. Here, we present a scalable in-situ thermal evaporation technique for synthesizing series of Bi, In, and Sn nanofilms on carbon felt (CF) substrates with a high-aspect-ratio structure. The resulting main-group metal nanofilms exhibit a homogeneously distributed and highly exposed catalyst surface with ample active sites, thereby promoting mass transport and ad-/desorption of reaction intermediates. Benefiting from the unique fractal morphology, the Bi nanofilms deposited on CF exhibit optimal catalytic activities for CO₂ electroreduction among the designed metal nanofilms electrodes, with the highest Faradaic efficiency of 96.9% for formate production at −1.3 V vs. reversible hydrogen electrode (RHE) in H-cell. Under an industrially relevant current density of 221.4 mA·cm⁻² in flow cells, the Bi nanofilms retain a high Faradaic efficiency of 81.7% at −1.1 V (vs. RHE) and a good long-term stability for formate production. Furthermore, a techno-economic analysis (TEA) model shows the potential commercial viability of electrocatalytic CO₂ conversion into formate using the Bi nanofilms catalyst. Our results offer a green and convenient approach for in-situ fabrication of stable and inexpensive thin-film catalysts with a fractal structure applicable to various industrial settings.

Throughout years, the two-step spin-coating process is the most common method to prepare organic lead halide perovskite materials. However, the short reaction time of dropping the solution at the second step means that PbI₂ cannot be completely transformed into perovskite phase. To solve this problem, we report the introduction of glycine hydrochloride (GlyHCl) into the second step of the two-step spin-coating process to prepare a FA_0.9MA_0.1PbI₃-x%-GlyHCl perovskite material (namely FAMA-x%-GlyHCl, where FA = formamidinium, MA = methylammonium, and x% stands for the molar ratio of GlyHCl added in FA iodide/MA iodide (FAI/MAI) precursor solution). The Cl⁻ ion in GlyHCl assists the formation of α-phase perovskite, and the –COO⁻ group coordinates with Pb²⁺ cation in a bridging way, making up for the anion vacancy in perovskite lattice and resulting in high absorption intensity. The perovskite solar cells (PSCs) based on FAMA-9%-GlyHCl achieve a long carrier lifetime (527.0 ns), a photoelectric conversion efficiency (PCE) of 19.40% and good thermal stability, maintaining 85.8% of the initial PCE after being continuously heated at 60 °C for 500 h. This study helps to solve the problem of incomplete reaction in the two-step spin-coating process and puts forward a new solution for preparing high coverage perovskite films with large grain size.

All-inorganic perovskites, adopting cesium (Cs⁺) cation to completely replace the organic component of A-sites of hybrid organic–inorganic halide perovskites, have attracted much attention owing to the excellent thermal stability. However, all-inorganic iodine-based perovskites generally exhibit poor phase stability in ambient conditions. Herein, we propose an efficient strategy to introduce antimony (Sb³⁺) into the crystalline lattices of CsPbI₂Br perovskite, which can effectively regulate the growth of perovskite crystals to obtain a more stable perovskite phase. Due to the much smaller ionic radius and lower electronegativity of trivalent Sb³⁺ than those of Pb²⁺, the Sb³⁺ doping can decrease surface defects and suppress charge recombination, resulting in longer carrier lifetime and negligible hysteresis. As a result, the all-inorganic perovskite solar cells (PSCs) based on 0.25% Sb³⁺ doped CsPbI₂Br light absorber and screen-printable nanocarbon counter electrode achieved a power conversion efficiency of 11.06%, which is 16% higher than that of the control devices without Sb³⁺ doping. Moreover, the Sb³⁺ doped all-inorganic PSCs also exhibited greatly improved endurance against heat and moisture. Due to the use of low-cost and easy-to-process nanocarbon counter electrodes, the manufacturing process of the all-inorganic PSCs is very convenient and highly repeatable, and the manufacturing cost can be greatly reduced. This work offers a promising approach to constructing high-stability all-inorganic PSCs by introducing appropriate lattice doping.

The electrocatalytic CO₂ reduction reaction (CO₂RR) is regarded as a promising route for renewable energy conversion and storage, but its development is limited by the high overpotential and low stability and selectivity of electrocatalysts. Moreover, it is complicated to accurately adjust the nanostructure of electrocatalysts, which impacts repeatability. Herein, we propose the rational design and controlled preparation of ultrafine Ag nanodots decorated fish-scale-like Zn nanoleaves (Ag-NDs/Zn-NLs) for highly selective electrocatalytic CO₂ reduction. The Ag-NDs/Zn-NLs can be in-situ grown on copper foil with simple electrodeposition and replacement reactions. Benefiting from the coordination and synergistic effect of Zn and Ag species, the reconstruction of Zn surface and the agglomeration of Ag-NDs are efficiently prevented, bringing high activity and durable electrocatalytic stability for CO₂-to-CO conversion. The Faradaic efficiency for CO production reaches 85.2% at a moderate applied potential of –1.0 V vs. reversible hydrogen electrode (RHE). This study provides a promising approach for controlling the catalytic activity and selectivity of CO₂RR through the structural adjustment and decoration of transition metal based nanocatalysts.

Silicon anodes have been extensively studied as a potential alternative to graphite ones for Li-ion batteries. However, their commercial application is limited by the issues of the poor structural and interfacial stability. In this regard, one of the key strategies for fully exploiting the capacity potential of Si-based anodes is to design robust conductive binder networks. Although the amount of binder in the electrode is small, it is, however, considered as a critical component of Si-based anodes for Li-ion batteries. In this review, a brief summary is given from the structural and functional aspects of the existing binders for Si anodes. In particular, three-dimensional and multifunctional polymeric binders with excellent electrical conductivity, flexibility, and adhesion prepared by chemical bonding, electrostatic and coordination interactions have become the focus of research, and are expected to accelerate the practical application of silicon anodes. Lastly, some suggestions for the future development of Si anodic binders are put forward.

Organic–inorganic metal halide perovskites have attained extensive attention owing to their outstanding photovoltaic performances, but the existence of numerous defects in crystalline perovskites is still a serious constraint for the further development of perovskite solar cells (PSCs). In particular, the rapid crystallization guided by anti-solvents leads to plenty of surficial and interfacial defects in perovskite films. Herein, we report the adoption of a pseudo-halide anion based ionic liquid additive, 1-butyl-3-methylimidazolium thiocyanate (BMIMSCN) for growing ternary cation (CsFAMA, where FA = formamidinium and MA = methylammonium) perovskites with large-scale crystal grains and strong preferential orientation via the enhanced Ostwald ripening. Meanwhile, a novel halide-free passivator, benzylammonium formate (BAFa), was employed as a buffering layer on the perovskite films to suppress surface-dominated charge recombination. As a result, the cooperative effects of BMIMSCN additive and BAFa passivator lead to significant enhancements on fluorescence lifetime (from 79.41 to 201.01 ns), open-circuit voltage (from 1.13 to 1.19 V), and photoelectric conversion efficiency (from 18.90% to 22.33%). Moreover, the BMIMSCN/BAFa-CsFAMA PSCs demonstrated greatly improved stability against moisture and heat. This work suggests a promising strategy to improve the quality of perovskite materials via reducing the surficial and interfacial defects by the synergistic effects of lattice doping and interface engineering.

Electrocatalytic carbon dioxide (CO₂) reduction is considered as an economical and environmentally friendly approach to neutralizing and recycling greenhouse gas CO₂. However, the design of preeminent and robust electrocatalysts for CO₂ electroreduction is still challenging. Herein, we report the in-situ growth of dense CuO_x nanowire forest on 3D porous Cu foam (CuO_x-NWF@Cu-F), which can be directly applied as a freestanding and binder-free working electrode for highly effective electrocatalytic CO₂ reduction. By adjusting the surface morphology and chemical composition of CuO_x nanowires via surface reconstruction, large electrochemically active surface area and abundant Cu(+1) sites were generated, leading to remarkable activity for CO₂ electroreduction. The as-prepared hierarchical conductive electrode exhibited an enhanced Faradaic efficiency of 15.0% for ethanol formation (FE_C2H5OH) and a total Faradaic efficiency of 69.4% for all carbonaceous compounds (FE_C-total) at a mild applied potential of –0.45 V vs. RHE in 0.1 M KHCO₃ electrolyte. It achieved a 4-fold increase in FE_C-total than that of Cu nanowire forest supported on 3D porous Cu foam (Cu-NWF@Cu-F) obtained by in-situ reduction of the CuO_x-NWF@Cu-F via annealing at H₂ atmosphere, and thereby effectively suppressed the hydrogen evolution side-reaction.

Rechargeable magnesium batteries are attractive candidates for energy storage due to their high theoretical specific capacities, free of dendrite formation and natural abundance of magnesium. However, the development of magnesium secondary batteries is severely limited by the lack of high-performance cathode materials and the incompatibility of electrode materials with electrolytes. Herein, we report the application of CuS nanoflower cathode material based on the conversion reaction mechanism for highly reversible magnesium batteries with boosted electrochemical performances by adjusting the compatibility between the cathode and electrolyte. By applying non-nucleophilic electrolytes based on magnesium bis(hexamethyldisilazide) and magnesium chloride dissolved in the mixed solvent of tetrahydrofuran and N-butyl-N-methyl-piperidinium bis((trifluoromethyl)sulfonyl)imide (Mg(HMDS)₂-MgCl₂/THF-PP₁₄TFSI) or magnesium bis(trifluoromethanesulfonyl)imide, magnesium chloride and aluminium chloride dissolved in dimethoxyethane (Mg(TFSI)₂-MgCl₂-AlCl₃/DME), the magnesium batteries with CuS nanoflower cathode exhibit a high discharge capacity of ~207 mAh·g^–1 at 100 mA·g^–1 and a long life span of 1,000 cycles at 500 mA·g^–1. This work suggests that the rational regulation of compatibility between electrode and electrolyte plays a very important role in improving the performance of multi-valent ion secondary batteries.

Photothermal carbon dioxide hydrogenation represents a promising route to reduce the emission of greenhouse gas CO₂ and produce value-added chemicals, but the selectivity and stability of photothermal catalysts need to be improved. Herein, we report the rational fabrication of well-defined Ag₂₄Au cluster decorated highly ordered nanorod-like mesoporous Co₃O₄ (Ag₂₄Au/meso-Co₃O₄) for highly efficient and selective CO₂ hydrogenation. The orderly assembled meso-Co₃O₄ nanorods were prepared via a nanocasting method, offering large surface area and abundant active sites for CO₂ adsorption and conversion. Moreover, the catalytic activity and selectivity were further improved by molecule-like Ag₂₄Au cluster decoration and reaction temperature optimization. The Ag₂₄Au/meso-Co₃O₄ composite catalyst exhibited an ultrahigh CH₄ yield rate of 204 mmol·g⁻¹·h⁻¹ and a greatly improved CH₄ selectivity of 82% for CO₂ hydrogenation, significantly higher than those of pristine meso-Co₃O₄ catalyst. The mechanism of the photothermal catalytic performance improvement was verified by CO₂ temperature-programmed desorption and time-resolved transient photoluminescence, revealing that CO₂ molecules underwent a vigorous adsorption and rapid activation process over Ag₂₄Au/meso-Co₃O₄. The hot electrons created by the localized surface plasmon resonance effect of Ag₂₄Au clusters facilitated the charge transfer for subsequent multi-electron CO₂ hydrogeneration processes, resulting in a significant increase in the productivity and selectivity for CO₂-to-CH₄ conversion. This work suggests that the rational coupling of well-defined metal atom clusters and ordered transition metal compound nanostructures could open a new avenue towards photo-induced green chemistry processes for efficient CO₂ recycling and reutilization.

The ultrahigh specific energy density and low cost of lithium-sulfur batteries are suitable for the next generation of energy storage. However, the shuttle issue and sluggish conversion kinetics of polysulfides remain unsolved. Confining metal nanoclusters with strong polarity in conductive porous carbon is an effective strategy for tackling such knotty issues. Herein, we design and synthesize hollow cubic carbon embedded with highly dispersed cobalt nanoclusters as an effective sulfur reservoir for lithium sulfur batteries. The large cavity structure and well-dispersed cobalt nanoclusters, with uniform sizes near 11 nm, enable the hosting structure to hold the high sulfur loading, 70% capacity retention after 500 cycles at 2 C with a high sulfur loading of 6.5 mg·cm⁻², effective stress release, accelerated polysulfide conversion, superior rate performance, strong physical confinement and chemical absorption capability. Further density functional theoretical calculations demonstrate that the well-dispersed cobalt nanoclusters in the hosting structure play a critical electrocatalytic role in boosting the capability of absorbing and converting polysulfides.