The rational design of efficient bimetallic nanoparticle (NP) catalysts is challenging due to the lack of theoretical understanding of active components and insights into the mechanisms of a specific reaction. Here, we report the rational design of nanoreactors comprising hollow carbon sphere-confined PtNi bimetallic NPs (PtNi@HCS) as highly efficient catalysts for hydrogen generation via ammonia borane hydrolysis in water. Using both density functional theory calculations and molecular dynamics simulations, the effects of an active PtNi combination and the critical synergistic role of a hollow carbon shell on the molecule diffusion adsorption behaviors are explored. Kinetic isotope effects and theoretical calculations allow the clarification of the mechanism, with oxidative addition of an O–H bond of water to the catalyst surface being the rate-determining step. The remarkable catalytic activity of the PtNi@HCS nanoreactor was also utilized for successful tandem catalytic hydrogenation reactions, using in situ-generated H₂ from ammonia borane with high efficiency. The concerted design, theoretical calculations, and experimental work presented here shed light on the rational elaboration of efficient nanocatalysts and contribute to the establishment of a circular carbon economy using green hydrogen.

Herein, Co/CoO heterojunction nanoparticles (NPs) rich in oxygen vacancies embedded in mesoporous walls of nitrogen-doped hollow carbon nanoboxes coupled with nitrogen-doped carbon nanotubes (P–Co/CoO_V@NHCNB@NCNT) are well designed through zeolite-imidazole framework (ZIF-67) carbonization, chemical vapor deposition, and O₂ plasma treatment. As a result, the three-dimensional NHCNBs coupled with NCNTs and unique heterojunction with rich oxygen vacancies reduce the charge transport resistance and accelerate the catalytic reaction rate of the P–Co/CoO_V@NHCNB@NCNT, and they display exceedingly good electrocatalytic performance for oxygen reduction reaction (ORR, halfwave potential [E_{ORR, 1/2} = 0.855 V vs. reversible hydrogen electrode]) and oxygen evolution reaction (OER, overpotential (η_OER, ₁₀ = 377 mV@10 mA cm^–2), which exceeds that of the commercial Pt/C + RuO₂ and most of the formerly reported electrocatalysts. Impressively, both the aqueous and flexible foldable all-solid-state rechargeable zinc–air batteries (ZABs) assembled with the P–Co/CoO_V@NHCNB@NCNT catalyst reveal a large maximum power density and outstanding long-term cycling stability. First-principles density functional theory calculations show that the formation of heterojunctions and oxygen vacancies enhances conductivity, reduces reaction energy barriers, and accelerates reaction kinetics rates. This work opens up a new avenue for the facile construction of highly active, structurally stable, and cost-effective bifunctional catalysts for ZABs.

Lithium metal batteries with inorganic solid-state electrolytes have emerged as strong and attractive candidates for electrochemical energy storage devices because of their high-energy content and safety. Nonetheless, inherent challenges of deleterious lithium dendrite growth and poor interfacial stability hinder their commercial application. Herein, we report a liquid metal-coated lithium metal (LM@Li) anode strategy to improve the contact between lithium metal and a Li₆PS₅Cl inorganic electrolyte. The LM@Li symmetric cell shows over 1000 h of stable lithium plating/stripping cycles at 2 mA cm^–2 and a significantly higher critical current density of 9.8 mA cm^–2 at 25°C. In addition, a full battery assembled with a high-capacity composite LiNbO₃@LiNi_0.7Co_0.2Mn_0.1O₂ (LNO@NCM721) cathode shows stable cycling performance. Experimental and computational results have demonstrated that dendrite growth tolerance and physical contact in solid-state batteries can be reinforced by using LM interlayers for interfacial modification.

A conventional electrode composite for rechargeable zinc-ion batteries (ZIBs) includes a binder for strong adhesion between the electrode material and the current collector. However, the introduction of a binder leads to electrochemical inactivity and low electrical conductivity, resulting in the decay of the capacity and a low rate capability. We present a binder- and conducting agent-free VO₂ composite electrode using in situ polymerization of dopamine on a flexible current collector of pyroprotein-based fibers. The as-fabricated composite electrode was used as a substrate for the direct growth of VO₂ as a self-supported form on polydopamine-derived pyroprotein-based fibers (pp-fibers@VO₂(B)). It has a high conductivity and flexible nature as a current collector and moderate binding without conventional binders and conducting agents for the VO₂(B) cathode. In addition, their electrochemical mechanism was elucidated. Their energy storage is induced by Zn²⁺/H⁺ coinsertion during discharging, which can be confirmed by the lattice expansion, the formation of by-products including Zn_x(OTf)_y(OH)_2x–y·nH₂O, and the reduction of V⁴⁺ to V³⁺. Furthermore, the assembled Zn//pp-fibers@VO₂(B) pouch cells have excellent flexibility and stable electrochemical performance under various bending states, showing application possibilities for portable and wearable power sources.

The successful utilization of an eco-friendly and biocompatible parylene-C substrate for high-performance solution-processed double-walled carbon nanotube (CNT) electrode-based perovskite solar cells (PSCs) was demonstrated. Through the use of a novel inversion transfer technique, vertical separation of the binders from the CNTs was induced, rendering a stronger p-doping effect and thereby a higher conductivity of the CNTs. The resulting foldable devices exhibited a power conversion efficiency of 18.11%, which is the highest reported among CNT transparent electrode-based PSCs to date, and withstood more than 10,000 folding cycles at a radius of 0.5 mm, demonstrating unprecedented mechanical stability. Furthermore, solar modules were fabricated using entirely laser scribing processes to assess the potential of the solution-processable nanocarbon electrode. Notably, this is the only one to be processed entirely by the laser scribing process and to be biocompatible as well as eco-friendly among the previously reported nonindium tin oxide-based perovskite solar modules.

Batteries that utilize low-cost elemental sulfur and light metallic lithium as electrodes have great potential in achieving high energy density. However, building a lithium–sulfur (Li–S) full battery by controlling the electrolyte volume generally produces low practical energy because of the limited electrochemical Li–S redox. Herein, the high energy/high performance of a Li–S full battery with practical sulfur loading and minimum electrolyte volume is reported. A unique hybrid architecture configured with Ni–Co metal alloy (NiCo) and metal oxide (NiCoO₂) nanoparticles heterogeneously anchored in carbon nanotube-embedded self-standing carbon matrix is fabricated as a host for sulfur. This work demonstrates the considerable improvement that the hybrid structure’s high conductivity and satisfactory porosity promote the transport of electrons and lithium ions in Li–S batteries. Through experimental and theoretical validations, the function of NiCo and NiCoO₂ nanoparticles as an efficient polysulfide mediator is established. These particles afford polysulfide anchoring and catalytic sites for Li–S redox reaction, thus improving the redox conversion reversibility. Even at high sulfur loading, the nanostructured Ni–Co metal alloy and metal oxide enable to have stable cycling performance under lean electrolyte conditions both in half-cell and full-cell batteries using a graphite anode.

A novel polybenzimidazole (PBI)-based trilayer membrane assembly is developed for application in vanadium redox flow battery (VRFB). The membrane comprises a 1 µm thin cross-linked poly[2,2’-(p-oxydiphenylene)–5,5’-bibenzimidazole] (OPBI) sandwiched between two 20 µm thick porous OPBI membranes (p-OPBI) without further lamination steps. The trilayer membrane demonstrates exceptional properties, such as high conductivity and low area-specific resistance (ASR) of 51 mS cm^–1 and 81 mΩ cm², respectively. Contact with vanadium electrolyte increases the ASR of trilayer membrane only to 158 mΩ cm², while that of Nafion is 193 mΩ cm². VO²⁺ permeability is 2.73 × 10^–9 cm² min^–1, about 150 times lower than that of Nafion NR212. In addition, the membrane has high mechanical strength and high chemical stability against VO₂⁺. In VRFB, the combination of low resistance and low vanadium permeability results in excellent performance, revealing high Coulombic efficiency (>99%), high energy efficiency (EE; 90.8% at current density of 80 mA cm^–2), and long-term durability. The EE is one of the best reported to date.

Exploiting high-performance yet low-cost hard carbon anodes is crucial to advancing the state-of-the-art sodium-ion batteries. However, the achievement of superior initial Coulombic efficiency (ICE) and high Na-storage capacity via low-temperature carbonization remains challenging due to the presence of tremendous defects with few closed pores. Here, a facile hybrid carbon framework design is proposed from the polystyrene precursor bearing distinct molecular bridges at a low pyrolysis temperature of 800°C via in situ fusion and embedding strategy. This is realized by integrating triazine- and carbonyl-crosslinked polystyrene nanospheres during carbonization. The triazine crosslinking allows in situ fusion of spheres into layered carbon with low defects and abundant closed pores, which serves as a matrix for embedding the well-retained carbon spheres with nanopores/defects derived from carbonyl crosslinking. Therefore, the hybrid hard carbon with intimate interface showcases synergistic Na ions storage behavior, showing an ICE of 70.2%, a high capacity of 279.3 mAh g^–1, and long-term 500 cycles, superior to carbons from the respective precursor and other reported carbons fabricated under the low carbonization temperature. The present protocol opens new avenues toward low-cost hard carbon anode materials for high-performance sodium-ion batteries.

The unique structural features of hard carbon (HC) make it a promising anode candidate for sodium-ion batteries (SIB). However, traditional methods of preparing HC require special equipment, long reaction times, and large energy consumption, resulting in low throughputs and efficiency. In our contribution, a novel synthesis method is proposed, involving the formation of HC nanosheets (NS-CNs) within minutes by creating an anoxic environment through flame combustion and further introducing sulfur and nitrogen sources to achieve heteroatom doping. The effect of heterogeneous element doping on the microstructure of HC is quantitatively analyzed by high-resolution transmission electron microscopy and image processing technology. Combined with density functional theory calculation, it is verified that the functionalized HC exhibits stronger Na⁺ adsorption ability, electron gain ability, and Na⁺ migration ability. As a result, NS-CNs as SIB anodes provide an ultrahigh reversible capacity of 542.7 mAh g^–1 at 0.1 A g^–1, and excellent rate performance with a reversible capacity of 236.4 mAh g^–1 at 2 A g^–1 after 1200 cycles. Furthermore, full cell assembled with NS-CNs as the can present 230 mAh g^–1 at 0.5 A g^–1 after 150 cycles. Finally, in/ex situ techniques confirm that the excellent sodium storage properties of NS-CNs are due to the construction of abundant active sites based on the novel synthesis method for realizing the reversible adsorption of Na⁺. This work provides a novel strategy to develop novel carbons and gives deep insights for the further investigation of facile preparation methods to develop high-performance carbon anodes for alkali-ion batteries.

Mo₂C is an excellent electrocatalyst for hydrogen evolution reaction (HER). However, Mo₂C is a poor electrocatalyst for oxygen evolution reaction (OER). Herein, two different elements, namely Co and Fe, are incorporated in Mo₂C that, therefore, has a finely tuned electronic structure, which is not achievable by incorporation of any one of the metals. Consequently, the resulting electrocatalyst Co_0.8Fe_0.2–Mo₂C-80 displayed excellent OER catalytic performance, which is evidenced by a low overpotential of 214.0 (and 246.5) mV to attain a current density of 10 (and 50) mA cm^–2, an ultralow Tafel slope of 38.4 mV dec^–1, and long-term stability in alkaline medium. Theoretical data demonstrates that Co_0.8Fe_0.2–Mo₂C-80 requires the lowest overpotential (1.00 V) for OER and Co centers to be the active sites. The ultrahigh catalytic performance of the electrocatalyst is attributed to the excellent intrinsic catalytic activity due to high Brunauer–Emmett–Teller specific surface area, large electrochemically active surface area, small Tafel slope, and low charge-transfer resistance.

This study attempts to develop a reproducible thin-film formation technique called vacuum-free (VF) lamination, which transfers thin films using elastomeric polymer-based laminating mediators. Precisely, by controlling the interface characteristics of the mediator based on the work of adhesion, VF lamination is successfully performed for various thicknesses (from 20 to 240 nm) of a conjugated photoactive material composed of poly[(2,6-(4,8-bis(5-(2-ethylhexyl-3-fluoro)thiophen-2-yl)-benzo[1,2-b:4,5-b′]dithiophene))-alt-(5,5-(1′,3′-di-2-thienyl-5′,7′-bis(2-ethylhexyl)benzo[1′,2′-c:4′,5′-c′]dithiophene-4,8-dione)] (a polymer donor) and 2,2′-((2Z,2′Z)-((12,13-bis(2-butyloctyl)-3,9-diundecyl-12,13-dihydro-[1,2,5]thiadiazolo[3,4-e]thieno[2′′,3′′:4′,5′]thieno[2′,3′:4,5]pyrrolo[3,2-g]thieno[2′,3′:4,5]thieno[3,2-b]indole-2,10-diyl)bis(methanylylidene))bis(5,6-difluoro-3-oxo-2,3-dihydro-1H-indene-2,1-diylidene))dimalononitrile (a nonfullerene acceptor). Interestingly, the organic photovoltaic and photodetecting applications, prepared by the VF lamination process, showed superior performance compared to those of devices prepared by conventional spin-coating. This is due to the overturned surface morphology, which led to enhanced charge transport ability and blocking of the externally injected charge. Thus, the reproducible VF lamination process, exploiting an adhesion-based elastomeric polymer mediator, is a promising thin-film formation technique for developing efficient next-generation organic optoelectronic materials consistent with the solution process.

Recent technological advancements, such as portable electronics and electric vehicles, have created a pressing need for more efficient energy storage solutions. Lithium-ion batteries (LIBs) have been the preferred choice for these applications, with graphite being the standard anode material due to its stability. However, graphite falls short of meeting the growing demand for higher energy density, possessing a theoretical capacity that lags behind. To address this, researchers are actively seeking alternative materials to replace graphite in commercial batteries. One promising avenue involves lithium-alloying materials like silicon and phosphorus, which offer high theoretical capacities. Carbon–silicon composites have emerged as a viable option, showing improved capacity and performance over traditional graphite or pure silicon anodes. Yet, the existing methods for synthesizing these composites remain complex, energy-intensive, and costly, preventing widespread adoption. A groundbreaking approach is presented here: the use of a laser writing strategy to rapidly transform common organic carbon precursors and silicon blends into efficient “graphenic silicon” composite thin films. These films exhibit exceptional structural and energy storage properties. The resulting three-dimensional porous composite anodes showcase impressive attributes, including ultrahigh silicon content, remarkable cyclic stability (over 4500 cycles with ˜40% retention), rapid charging rates (up to 10 A g^–1), substantial areal capacity (>5.1 mAh cm^–2), and excellent gravimetric capacity (>2400 mAh g^–1 at 0.2 A g^–1). This strategy marks a significant step toward the scalable production of high-performance LIB materials. Leveraging widely available, cost-effective precursors, the laser-printed “graphenic silicon” composites demonstrate unparalleled performance, potentially streamlining anode production while maintaining exceptional capabilities. This innovation not only paves the way for advanced LIBs but also sets a precedent for transforming various materials into high-performing electrodes, promising reduced complexity and cost in battery production.

Platinum-based alloy nanoparticles are the most attractive catalysts for the oxygen reduction reaction at present, but an in-depth understanding of the relationship between their short-range structural information and catalytic performance is still lacking. Herein, we present a synthetic strategy that uses transition-metal oxide-assisted thermal diffusion. PtCo/C catalysts with localized tetragonal distortion were obtained by controlling the thermal diffusion process of transition-metal elements. This localized structural distortion induced a significant strain effect on the nanoparticle surface, which further shortened the length of the Pt–Pt bond, improved the electronic state of the Pt surface, and enhanced the performance of the catalyst. PtCo/C catalysts with special short-range structures achieved excellent mass activity (2.27 A mg_Pt^–1) and specific activity (3.34 A cm^–2). In addition, the localized tetragonal distortion-induced surface compression of the Pt skin improved the stability of the catalyst. The mass activity decreased by only 13% after 30,000 cycles. Enhanced catalyst activity and excellent durability have also been demonstrated in the proton exchange membrane fuel cell configuration. This study provides valuable insights into the development of advanced Pt-based nanocatalysts and paves the way for reducing noble-metal loading and increasing the catalytic activity and catalyst stability.

Hydrogen (H₂) has been regarded as a promising alternative to fossil-fuel energy. Green H₂ produced via water electrolysis (WE) powered by renewable energy could achieve a zero-carbon footprint. Considerable attention has been focused on developing highly active catalysts to facilitate the reaction kinetics and improve the energy efficiency of WE. However, the stability of the electrocatalysts hampers the commercial viability of WE. Few studies have elucidated the origin of catalyst degradation. In this review, we first discuss the WE mechanism, including anodic oxygen evolution reaction (OER) and cathodic hydrogen evolution reaction (HER). Then, we provide strategies used to enhance the stability of electrocatalysts. After that, the deactivation mechanisms of the typical commercialized HER and OER catalysts, including Pt, Ni, RuO₂, and IrO₂, are summarized. Finally, the influence of fluctuating energy on catalyst degradation is highlighted and in situ characterization methodologies for understanding the dynamic deactivation processes are described.

Diamond possesses excellent thermal conductivity and tunable bandgap. Currently, the high-pressure, high-temperature, and chemical vapor deposition methods are the most promising strategies for the commercial-scale production of synthetic diamond. Although diamond has been extensively employed in jewelry and cutting/grinding tasks, the realization of its high-end applications through microstructure engineering has long been sought. Herein, we discuss the microstructures encountered in diamond and further concentrate on cutting-edge investigations utilizing electron microscopy techniques to illuminate the transition mechanism between graphite and diamond during the synthesis and device constructions. The impacts of distinct microstructures on the electrical applications of diamond, especially the photoelectrical, electrical, and thermal properties, are elaborated. The recently reported elastic and plastic deformations revealed through in situ microscopy techniques are also summarized. Finally, the limitations, perspectives, and corresponding solutions are proposed.