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Acidic CO2 electrolysis offers a promising strategy to achieve high carbon utilization and high energy efficiency. However, challenges still remain in suppressing the competitive hydrogen evolution reaction (HER) and improving product selectivity. Although high concentrations of potassium ions (K+) can suppress HER and accelerate CO2 reduction, they still inevitably suffer from salt precipitation problems. In this study, we demonstrate that the sulfonate‐based polyelectrolyte, polystyrene sulfonate (PSS), enables to reconstruct the electrode‐electrolyte interface to significantly enhance the acidic CO2 electrolysis. Mechanistic studies reveal that PSS induces high local K+ concentrations through the electrostatic interaction between PSS anions and K+. In situ spectroscopy reveals that PSS reshapes the interfacial hydrogen–bond (H‐bond) network, which is attributed to the H‐bonds between PSS anions and hydrated proton, as well as the steric hindrance of the additive molecules. This greatly weakens proton transfer kinetics and leads to the suppression of undesirable HER. As a result, a Faradaic efficiency of 93.9 % for CO can be achieved at 250 mA cm−2, simultaneous with a high single‐pass carbon efficiency of 72.2 % on commercial Ag catalysts in acid. This study highlights the important role of the electrode‐electrolyte interface induced by polyelectrolyte additives in promoting electrocatalytic reactions. [ABSTRACT FROM AUTHOR]

Highly‐dispersed single‐crystalline Ni‐rich cathodes with low Li/O loss are the key for high‐power Li‐ion batteries, but it is still a big challenge because an additional 60–110 °C higher synthesis temperature is required in comparison with the polycrystalline counterparts. Herein, a highly‐ordered and monodisperse single‐crystalline LiNi0.83Co0.12Mn0.05O2 (NCM83) cathode with an average size of 3.24 µm is reported by a Sr/Nb synergically controlling the grain surface energy strategy based on the Vegard's slopes of various ions. The solid‐phase lithiation temperature is reduced by ≈80 °C, greatly reducing Li/Ni disorder and oxygen vacancies with rapid Li‐ion diffusion kinetics and high structure stability. The introduced Sr/Nb ions remarkably increase the electron cloud density near the Fermi level, while alleviating the H2‐H3 phase transition with reduced lattice shrinkage. The as‐prepared single‐crystalline NCM83 cathode exhibits obvious increased capacity retention of 60% at 10C (vs. 0.1C) in coin‐type half‐cells and 89% after cycling 1000 times at 0.5C in pouch‐type full‐cells. The work sheds light on the low‐temperature synthesis of monodisperse and uniform single‐crystalline Ni‐rich cathodes for high‐power and long‐life Li‐ion batteries. [ABSTRACT FROM AUTHOR]

Bicarbonate electrolysis, as a carbon utilization technology with high efficiency and potential for industrial applications, provides a promising pathway for CO2 emission reduction. However, how to inhibit serious hydrogen evolution reaction (HER) and increase the relatively low CO2 concentration at the electrode‐electrolyte interfacial is challenging. Here, we introduce three typical aminopolycarboxylic acids (APCAs) with different amounts of carboxylic acid roots into 3 M KHCO3 to enhance the Faradaic efficiency of CO (FECO) from 51.2% to 68.0% at 100 mA cm−2. Spectroscopic characterization confirms that the role of APCAs in confining the activity of water dissociation and improving the availability of CO2. The strategy adopted in this work that introducing APCAs into the electrolyte to balance the content of CO2 and H2O for improving the electrocatalytic performance, can serve as a reference for other electrocatalytic systems. [ABSTRACT FROM AUTHOR]

Electrocatalytic semi‐hydrogenation of alkynols holds tremendous advantages over conventional thermocatalysis process. However, the selectivity‐activity seesaw effect is a principal obstacle to its further development. Inspired by interfacial self‐assembled monolayers, alkanethiols with different alkyl chain lengths are employed to modify the Cu surface for controllably modulating the activity and selectivity in the semi‐hydrogenation of alkynols. 1‐dodecanethiol‐modified Cu nanowires (Cu NWs) exhibit the optimal electrosynthesis of 2‐methyl‐3‐buten‐2‐ol with excellent specific selectivity (above 93%) in the semi‐hydrogenation of 2‐methyl‐3‐butyn‐2‐ol. Mechanistic studies reveal that the proportion of liquid‐like water increases while the proportion of isolated water reduces at the hydrophobic interface. Moreover, we assemble a larger 3 × 100 cm2 electrolyzer stack, which can deliver a single‐pass alkynol conversion rate of 95% and an excellent alkenol selectivity of 94% at a 15 A stack current. Eventually, the Cu NWs catalyst with thiol treatment is also applicable to the semi‐hydrogenation of various unsaturated alkynols. [ABSTRACT FROM AUTHOR]

While blending with flexible polymers has been a commonly employed strategy to enhance the toughness of polylactic acid (PLA), it's still a great challenge to avoid the sacrifice of tensile strength at the same time. In this work, we demonstrate a promising route to simultaneously improve the strength and toughness of PLA by compounding PLA with poly(ε‐caprolactone) (PCL) and PLA grafted multi‐walled carbon nanotubes core‐shell nanofiller (MWNT‐PCLPLA) via a two‐step ring‐opening polymerization and have analyzed the strengthening and toughening mechanism through molecular dynamics simulation. The double polymer layers of MWNT‐PCLPLA effectively improve the interfacial interaction between MWNTs and the matrix, in which the outer PLA layer has the same molecular structure with the matrix and facilitates stress transfer, while the flexible PCL layer can absorb energy through self‐deformation and induce local plastic deformation of the matrix. When the content of MWNTs was only 1 wt%, the strength and elongation at break of PLA/MWNT‐PCLPLA nanocomposites were increased by 47.92% and 690.11% compared to neat PLA. Furthermore, the toughness of nanocomposites reached 11.93 MJ/m3, which is about 16 times that of neat PLA. This novel core‐shell nanofiller with double polymer layers is expected to be further applied in other polymer systems. Highlights: A core‐shell nanofiller with double polymer layers was synthesized.Improved dispersion and interfacial compatibility of nanofillers in matrix.The crystallization ability of PLA was improved by functionalized MWNTs.Simultaneously improved strength and toughness of PLA/MWNT‐PCLPLA nanocomposite. [ABSTRACT FROM AUTHOR]

The synthesis of high‐entropy alloys (HEAs) with ultra‐small particle sizes has long been a challenging task. The complex and time‐consuming synthesis process hinders their practical application and widespread adoption. This study presents the novel synthesis of TiO2 nanoparticles loaded with a quinary high‐entropy alloy through flame spray pyrolysis (FSP) for the first time. The extremely fast heating rate of flame combustion makes the precursor fast pyrolysis gasification, high temperature in the flame field promotes the metal vapor mixing uniformly, and the fast quenching process can reduce the particle aggregation sintering, the ultra‐small particle size of HEA firmly attached to the TiO2 surface. The catalysts prepared via this gas‐to‐particle pathway exhibit excellent performance in CO2 hydrogenation, achieving a conversion rate of 62% at 450 °C, and maintaining their activity for over 220 h without significant particle agglomeration. This finding provides valuable insights for the future design of catalytically active materials with enhanced activity and long‐term stability. [ABSTRACT FROM AUTHOR]

Conventional strategies for highly selective and active hydrogen peroxide (H2O2) electrosynthesis primarily focus on catalyst design. Electrocatalytic reactions take place at the electrified electrode–electrolyte interface. Well‐designed electrolytes, when combined with commercial catalysts, can be directly applied to high‐efficiency H2O2 electrosynthesis. However, the role of electrolyte components is equally crucial but is significantly under‐researched. In this study, anionic surfactant n‐tetradecylphosphonic acid (TDPA) and its analogs are used as electrolyte additives to enhance the selectivity of the two‐electron oxygen reduction reaction. Mechanistic studies reveal that TDPA assembled over the electrode–electrolyte interface modulates the electrical double‐layer structure, which repels interfacial water and weakens the hydrogen‐bond network for proton transfer. Additionally, the hydrophilic phosphonate moiety affects the coordination of water molecules in the solvation shell, thereby directly influencing the proton‐coupled kinetics at the interface. The TDPA‐containing catalytic system achieves a Faradaic efficiency of H2O2 production close to 100% at a current density of 200 mA cm−2 using commercial carbon black catalysts. This research provides a simple strategy to enhance H2O2 electrosynthesis by adjusting the interfacial microenvironment through electrolyte design. [ABSTRACT FROM AUTHOR]

The practical application of lithium‐sulfur batteries with high theoretical energy density and readily available cathode active materials is hampered by problems such as sulfur insulation, dramatic volume changes, and polysulfide shuttling. The targeted development of novel binders is the most industrialized solution to the problem of sulfur cathodes. Herein, an aqueous conductive emulsion binder with the sulfonate‐containing hard elastic copolymer core and the conjugate polymer shell, which is capable of forming a bicontinuous mesoscopic interpenetrating polymer network, is synthesized and investigated. Not only can the elastic skeleton formed by the copolymer bind the active substance under drastic volume changes, but also the rich ester and cyanide groups in it can effectively capture lithium polysulfide. Meanwhile, the conducting skeleton consisting of poly(3,4‐ethylenedioxythiophene) both provides the additional charge conduction pathways and acts as the redox intermediates, significantly accelerating the kinetic process of lithium polysulfide conversion. Based on the synergistic effect of the above mechanisms, the use of the prepared binder on the sulfur carbon cathode significantly improves the rate performance and cycle stability of lithium sulfur batteries. [ABSTRACT FROM AUTHOR]

The electrochemical reduction of nitrates (NO3RR) for ammonia synthesis at room temperature holds immense potential. One key challenge is the adsorption and activation of NO3−, along with the provision of sufficient active hydrogen to accelerate the hydrogenation process. Here, the study prepares N‐doped TiO2‐x supported by Zr single atoms (Zr‐TiON) with rich oxygen vacancies (Ov), in which unsaturated Zr (Lewis acidic, LA) sites together with oxygen atoms around Ov (Lewis base, LB) form frustrated Lewis acid‐base pairs (FLPs). At −60 mA cm−2, NH3 Faradaic efficiency reaches 94.8%, corresponding to the production rate of 663.15 µmol h−1 mgcat−1. The yield rate is up to 26.16 mmol h−1mgcat−1 at −1 A cm−2 in flowing electrolyzer. Theoretical calculations and in situ spectroscopy analysis reveal that the interaction between LA and LB sites in FLPs plays a crucial role in facilitating adsorption and activation of electron‐rich NO3− and electron‐deficient *H. The presence of enhanced FLPs significantly reduces the energy barrier for H2O dissociation, lowering it to 0.20 eV, which facilitates subsequent hydrogenation reactions. The abundance of *H accelerates hydrogenation process, thereby enhancing the activity of NO3RR. This FLP design offers a promising approach for paving the way for the development of highly efficient NO3RR catalysts. [ABSTRACT FROM AUTHOR]

Carbon dioxide (CO2) electrolysis is an important process for storing excess renewable electricity. However, this process is commonly carried out in a high‐purity‐CO2 environment. Here, we conduct a systematic investigation into the operational performance of CO2 capture solutions for producing syngas. Using Ni‐N‐C electrocatalysts, by reducing the thickness of the catalytic layer and accelerating the mass transport, we achieve 58.6% CO Faradaic efficiency at a current density of 100 mA cm−2 and a full cell voltage of 3.67 V. Efficient syngas (MolH2/MolCO = 1–4) production has achieved at a wide range of current densities, that is, 100 to 300 mA cm−2 using a 3 M KHCO3 solution. It is also demonstrated that the Ni‐N‐C electrocatalysts compared to commercial Ag catalysts show better impurity tolerance and CO selectivity. These findings underscore the potential of CO2 capture solution as a direct carbon source for CO2 electrolysis. [ABSTRACT FROM AUTHOR]

Electrocatalytic hydrogenation of unsaturated aldehydes to unsaturated alcohols is a promising alternative to conventional thermal processes. Both the catalyst and electrolyte deeply impact the performance. Designing the electrode‐electrolyte interface remains challenging due to its compositional and structural complexity. Here, we employ the electrocatalytic hydrogenation of 5‐hydroxymethylfurfural (HMF) as a reaction model. The typical cationic surfactant, cetyltrimethylammonium bromide (CTAB), and its analogs are employed as electrolyte additives to tune the interfacial microenvironment, delivering high‐efficiency hydrogenation of HMF and inhibition of the hydrogen evolution reaction (HER). The surfactants experience a conformational transformation from stochastic distribution to directional assembly under applied potential. This oriented arrangement hampers the transfer of water molecules to the interface and promotes the enrichment of reactants. In addition, near 100 % 2,5‐bis(hydroxymethyl)furan (BHMF) selectivity is achieved, and the faradaic efficiency (FE) of the BHMF is improved from 61 % to 74 % at −100 mA cm−2. Notably, the microenvironmental modulation strategy applies to a range of electrocatalytic hydrogenation reactions involving aldehyde substrates. This work paves the way for engineering advanced electrode‐electrolyte interfaces and boosting unsaturated alcohol electrosynthesis efficiency. [ABSTRACT FROM AUTHOR]

CO2 electrolysis to value‐added chemicals and fuels shows tremendous potential to store renewable electricity. It features with H2O as the hydrogen source of CO2 electroreduction. Here, we aim at the effect of the hydrophobicity‐tuned catalyst microenvironment in gas diffusion electrode (GDE) on boosting CO2 electrolysis. The hydrophobic polytetrafluoroethylene (PTFE) nanoparticles are introduced in the Sn catalyst layer of GDE. The PTFE‐modified GDE compared to the non‐PTFE electrode delivers a higher HCOOH Faraday efficiency and lower overpotential at current densities of 50–250 mA cm−2. A two‐dimensional axisymmetric model jointly with electrochemical impedance spectroscopy is developed to provide mechanistic insights into the hydrophobicity regulation. The simulated polarization current densities are in keeping with experimental results. The boosted CO2 electrolysis is attributed to the decrease of the distance from the gas–liquid phase boundary to the electrocatalyst. The understanding of the catalyst microenvironment established here can be generalized to other gas‐involved electrocatalytic reactions. [ABSTRACT FROM AUTHOR]

Electrochemical acetonitrile hydrogenation compared with thermocatalytic hydrogenation provides a potential route to produce ethylamine in mild conditions. It is challenging to suppress the C–C coupling for improving ethylamine selectivity. Here, Ru‐supported Cu nanowire catalysts (Ru‐Cu NWs) are designed to achieve nearly 100% specific selectivity of ethylamine without coupling byproducts. In situ vibrational spectroscopy and electron spin resonance results reveal that the Ru‐Cu NWs provide a high active adsorption hydrogen (H*) coverage at the electrified interface so that the imine intermediates are more readily hydrogenated to generate ethylamine, thus suppressing the C–C coupling. Density functional theory calculations disclose that the formation of H* occurs more readily over Ru‐Cu NWs than Cu NWs. Moreover, the presence of Ru changes the potential‐determining step and facilitates the entire hydrogenation process. The strategy and understanding established here can be extended to other electrocatalytic hydrogenation reactions. [ABSTRACT FROM AUTHOR]

Copper oxide nanomaterials have been suggested to be efficient for highly selective multi‐carbon (C2+) production in CO2 reduction reaction (CO2RR), due to the introduction of surface Cu+ species from oxide catalysts. However, the Cu+ species on the catalyst surface are prone to being reduced to Cu0 under reductive conditions during CO2RR. Here, a network‐structured catalyst is developed consisting of ultrafine Cu2O/CuO nanoparticles that harbor an abundance of pores. This catalyst is synthesized via flame spray pyrolysis (FSP) method and engineered to confine carbon intermediates, which subsequently cover the local catalyst surface and stabilize Cu+ species. As a result, a C2+ products Faradaic efficiency (FE) of approximately 80.0% at a partial current density of 320.0 mA cm−2 is achieved, and a large C2+ to C1 ratio of ≈9.7. In situ XRD and XPS spectra are employed to reveal the indeed presence of Cu+ species on the catalyst surface during the CO2RR process, which extensively improves the adsorption of *CO intermediates and thus the C─C coupling reaction to form C2+ products. [ABSTRACT FROM AUTHOR]

The electrochemical nitrate reduction reaction (NO3RR) is an environment‐friendly and promising alternative to the conventional Haber–Bosch ammonia synthesis process, which is a complex process of proton‐coupled electron transfer. Hereon, the amorphous CeOx support introduced to construct Cu/a‐CeOx heterostructure is prepared to provide sufficient *H and synergistically catalyze the NO3RR. Cu/a‐CeOx achieves a maximum ammonia yield of 1.52 mmol h−1 mgcat−1. In the flow cell, the NH3 yield reaches 17.93 mmol h−1 mgcat−1 at 1 A cm−2, which exceeds most of the state‐of‐the‐art catalysts. In situ X‐ray diffraction (XRD) and in situ Raman observe that the catalyst undergoes structural reconfiguration under operating conditions, thus confirming that Cu2O is not the true active center in the catalytic process. Furthermore, in situ characterizations and density functional theory (DFT) calculations demonstrate that the amorphous CeOx in Cu/a‐CeOx modulates the electronic structure of Cu and overcomes the higher potential barrier required for the decomposition of water on Cu, which greatly facilitates the hydrolysis process and provides a higher H‐coverage rate for the hydrogenation of NO3−, realizing a dynamic equilibrium between the production and consumption of active hydrogen. This component design strategy centered on the amorphous structure opens up a new pathway for the electrochemical NO3RR. [ABSTRACT FROM AUTHOR]

All‐inorganic lead halide perovskite nanocrystals (NCs) have shown great potential in various optoelectronic device applications due to their excellent optoelectronic properties, but their poor stability remains a key obstacle to widespread application. The preparation of core/shell NCs is developed to improve their stability, but most of the coating for single NCs is incomplete, and the crystal orientation and interface binding of core/shell structures are still unclear. Here, a surface reconstruction strategy to synthesize CsPbBr3/CsPb2Br5 core/shell NCs with uniform coating structure is reported. The concentration of [PbBr8]6− monomer in the system is regulated by creating local low H2O concentration conditions to balance the erosion of perovskite by water and the overall heterogeneous nucleation reaction system, resulting in single encapsulated and well‐edged perovskite core/shell NCs. More importantly, advanced characterization tools are used to reveal the core/shell structural features of CsPbBr3/CsPb2Br5 core/shell NCs at the atomic scale, which has not been reported before, and the interface matching of the two‐phase binding is simulated by density functional theory calculations, which confirm that the CsPb2Br5 (116) facet can bind to the CsPbBr3 (100) facet with the lowest binding energy. The prepared core/shell perovskite NCs can still retain photoluminescence emission after >30 days in water. [ABSTRACT FROM AUTHOR]

Granulite facies metamorphism and crustal anatexis exist in the East Cathaysia Block, the exact timing of granulite facies partial melting and its link with orogenesis have not been well constrained. In this study, we carried out petrography, whole rock geochemistry, and zircon U–Pb dating, trace elements and Hf isotopes analyses on Dazhe gneissic granite and banded migmatite from the Badu Group in southwest Zhejiang province in the East Cathaysia Block. The melts were produced through the dehydration of biotite, such as biotite + quartz + plagioclase = orthopyroxene + K‐feldspar + melt and biotite + quartz + plagioclase + sillimanite = garnet + K‐feldspar + melt. Zircons from these rocks show clear core‐rim structure and yield rim and core concordant ages at 233 Ma and 1.83 Ga, respectively. The zircon rims suggesting the melts and the cores are suggesting the protolith of Dazhe gneissic granite and banded migmatite were crystallized from an evolving magma. The zircon cores and rims have negative εHf(t) = −2.2 ~ −6.3 and εHf(t) = −22.8 ~ −32.4, and they give suggestion of the presence of Neoarchean components. Although the major‐element compositions of the gneissic granite and banded migmatite are slightly different, the trace‐element spider diagram and REE pattern show they are similar, and then we find that the protoliths are A‐type granodiorite/diorite. Combined with the published data, we suggested that the Dazhe gneissic granite and banded migmatite were formed through granulite facies partial melting at 233 Ma, which was promoted by crustal shortening and thickening of the collision orogeny between East Cathaysia Block and an unknown terrane with a NNE trend structure line. The protoliths (granite or granodiorite) of Dazhe gneissic granite and banded migmatite crystallized at 1.83 Ga by reworking of the Neoarchean components of East Cathaysia Block. The Paleoproterozoic (1912–1819 Ma) collisional orogeny and the later intraplate rifting stage are corresponding to the aggregation and breakup of the Columbia supercontinent. [ABSTRACT FROM AUTHOR]

Cu‐based catalysts exhibit the unique ability to generate high‐order products from electrochemical CO2 reduction reaction (CO2RR). The performance of electrochemical systems is jointly influenced by the catalysts and local microenvironment of the electrode–electrolyte interface. Here, Cu nanowires as a model catalyst, in combination with cetyl trimethyl ammonium bromide (CTAB) as electrolyte additives, are designed to steer CO2RR. By using the Cu rotating disc electrode and in situ vibrational spectroscopy, it is revealed that the hydrophobic interface microenvironment is built, and the interaction of interfacial water and surface‐adsorbed CO is disrupted by CTAB, which dramatically improve formate selectivity (from 5% to 63%) with a high partial current density of formate (13‐fold increase) at −1.0 V vs. reversible hydrogen electrode. The understanding of the surfactant‐modified electrode–electrolyte interface established here offers a distinct perspective to control the microenvironment on promoting electrosynthesis performance. [ABSTRACT FROM AUTHOR]

The site isolation strategy has been employed in thermal catalytic acetylene semihydrogenation to inhibit overhydrogenation and C−C coupling. However, there is a dearth of analogous investigations in electrocatalytic systems. In this work, density functional theory (DFT) simulations demonstrate that isolated Cu metal sites have higher energy barriers on overhydrogenation and C−C coupling. Following this result, we develop Cu single‐atom catalysts highly dispersed on nitrogen‐doped carbon matrix, which exhibit high ethylene selectivity (>80 % Faradaic efficiency for ethylene, <1 % Faradaic efficiency for C4, and no ethane) at high concentrations of acetylene. The superior performance observed in the electrocatalytic selective hydrogenation of acetylene can be attributed to the weak adsorption of ethylene intermediates and highly energy barriers on C−C coupling at isolated sites, as confirmed by both DFT calculations and experimental results. This study provides a comprehensive understanding of the isolated sites inhibiting the side reactions of electrocatalytic acetylene semihydrogenation. [ABSTRACT FROM AUTHOR]

Designing highly efficient and stable electrode‐electrolyte interface for hydrogen peroxide (H2O2) electrosynthesis remains challenging. Inhibiting the competitive side reaction, 4 e− oxygen reduction to H2O, is essential for highly selective H2O2 electrosynthesis. Instead of hindering excessive hydrogenation of H2O2 via catalyst modification, we discover that adding a hydrogen‐bond acceptor, dimethyl sulfoxide (DMSO), to the KOH electrolyte enables simultaneous improvement of the selectivity and activity of H2O2 electrosynthesis. Spectral characterization and molecular simulation confirm that the formation of hydrogen bonds between DMSO and water molecules at the electrode‐electrolyte interface can reduce the activity of water dissociation into active H* species. The suitable H* supply environment hinders excessive hydrogenation of the oxygen reduction reaction (ORR), thus improving the selectivity of 2 e− ORR and achieving over 90 % selectivity of H2O2. This work highlights the importance of regulating the interfacial hydrogen‐bond environment by organic molecules as a means of boosting electrochemical performance in aqueous electrosynthesis and beyond. [ABSTRACT FROM AUTHOR]

The earth‐abundant hard carbons have drawn great concentration as potassium‐ion batteries (KIBs) anode materials because of their richer K‐storage sites and wider interlayer distance versus graphite, but suffer from a low electrochemical reversibility. Herein, the novel Se/N co‐doped hard‐carbon nanotubes (h‐CNTs) with localized electron configuration are demonstrated by creating unique NSeC covalent bonds stemmed from the precise doping of Se atoms into carbon edges and the subsequent bonding with pyrrole‐N. The strong electron‐donating ability of Se atoms on d‐orbital provides abundant free electrons to effectively relieve charge polarization of pyrrole‐N‐C bonds, which contributes to balance the K‐ion adsorption/desorption, therefore greatly boosting reversible K‐ion storage capacity. After filtering into self‐standing anodes with weights of 1.5–12.4 mg cm−2, all of them deliver a high reversible gravimetric capacity of 341 ± 4 mAh g−1 at 0.2 A g−1 and a linear increasing areal capacity to 4.06 mAh cm−2. The self‐standing anode can still maintain 209 mAh g−1 at 8.0 A g−1 (93.3% retention) for a long period of 2000 cycles with a constant Se/N content. [ABSTRACT FROM AUTHOR]

Supercapacitor represents an important electrical energy storage technology with high‐power performance and superior cyclability. However, currently commercialized supercapacitors still suffer limited energy densities. Here we report an unprecedentedly respiring supercapacitor with chlorine gas iteratively re‐inspires in porous carbon materials, that improves the energy density by orders of magnitude. Both electrochemical results and theoretical calculations show that porous carbon with pore size around 3 nm delivers the best chlorine evolution and adsorption performance. The respiring supercapacitor with multi‐wall carbon nanotube as the cathode and NaTi2(PO4)3 as the anode can store specific energy of 33 Wh kg−1 with negligible capacity loss over 30 000 cycles. The energy density can be further improved to 53 Wh kg−1 by replacing NaTi2(PO4)3 with zinc anode. Furthermore, thanks to the extraordinary reaction kinetics of chlorine gas, this respiring supercapacitor performs an extremely high‐power density of 50 000 W kg−1. [ABSTRACT FROM AUTHOR]

Electrochemical production of hydrogen peroxide (H2O2) from O2 on single‐atom catalysts has attracted great attention, yet the quest for robust catalysts is driven by achieving >90 % Faradaic efficiency (FE) under industrial‐relevant current densities (>100 mA cm−2). Herein we synthesize a catalyst that contains single nickel site coordinated by four nitrogen and two oxygen atoms (i.e. N4Ni1O2) via involving carboxyl functionalized multiwall carbon nanotubes as a substrate to provide extra O coordination to the regular NiN4 site. It has a cathodic energy efficiency of approximately 82 % and a H2O2 FE of around 96 % at 200 mA cm−2 current density, outperforming the reported single‐atom catalysts for H2O2 electrosynthesis. [ABSTRACT FROM AUTHOR]

Perovskite quantum dots (PQDs) have wide applications in optoelectronic devices due to their excellent stability and processability. However, PQD films are still seeking to overcome the problems of disorder and porosity. This seriously hinders the carrier transport and the application of PQDs in photodetectors (PDs). In this work, the electrophoretic deposition (EPD) method is employed to fabricate PQDs with conjugated linoleic acid (CLA) as the ligands, and the highly oriented and dense films are obtained. In addition, CLA molecules can polymerize during electrophoresis, which shortens the quantum dot spacing. It facilitates carrier transport while improving the stability of the film. PDs prepared by electrophoresis have a high detectivity (D*) up to 5.1 × 1012 Jones, which is 3.9 times higher than PDs prepared by spin coating (1.3 × 1012 Jones) and reaches the highest record under the same conditions. In addition, the device exhibits a remarkable stability, maintaining 95% of the initial performance when left in the air for 3 months. This work provides a new perspective on the assembly of PQDs in the application of optoelectronic devices. [ABSTRACT FROM AUTHOR]

To make up for the brittleness of poly(lactic acid) (PLA), people usually introduce flexible poly(butylene adipate‐co‐terephthalate) (PBAT) which greatly reduces the strength and limits toughening effect due to unfavorable immiscibility of the blends. Herein, functionalized biodegradable cellulose nanocrystals (CNCs) were used as enhancement to simultaneously improve strength and toughness of PLA/PBAT blend. To improve the interaction between PLA and PBAT, poly(glycidyl methacrylate) (PGMA) was grafted on the surface of CNC via a surface‐initiated atom transfer radical polymerization reaction. After the addition of CNC‐PGMA30, the phase size of PLA/PBAT (70/30 wt%) reduces dramatically, showing improved interfacial compatibility between PLA and PBAT. Meanwhile, prepared PLA/PBAT/CNC1.0‐PGMA30 composite has tensile strength of 49.6 MPa and elongation at break of 268.5%, demonstrating considerably increased strength and toughness in comparison to the pure PLA/PBAT blend. [ABSTRACT FROM AUTHOR]

The electrocatalytic nitrogen reduction reaction (NRR) for NH3 synthesis is still far from being practical and competitive with the common Haber–Bosch process. The rational design of highly selective NRR electrocatalyst is therefore urgently needed, which requires a deep understanding of both the electrode–electrolyte interface and the mass transport of reactants. Here, we develop a theoretical framework that includes electric double layer (EDL), mass transport, and the NRR kinetics. This allows us to evaluate the roles of near‐electrode environment and N2 diffusion on the NRR selectivity and activity. The EDL, as the immediate reaction environment, remarkably impedes the diffusion of N2 to the cathode surface at high electrode potentials, which explains experimental observations. This article also gives microscopic insights into the interplay between N2 diffusion and reaction activity under the nano‐confinement, providing theoretical guidance for future design of advanced NRR electrocatalytic systems. [ABSTRACT FROM AUTHOR]

Owing to the lower price and higher safety, developing high‐performance K‐ion batteries (KIBs) is of great significance as an alternative to Li‐ion batteries. High‐energy‐density MoSe2 has been identified as a promising anode material for KIBs; however, its electrochemical reversibility remains a big challenge. Herein, heterogenous MoSe2/N‐doped carbon nanoarrays demonstrate a brilliant performance as KIBs anode materials. The as‐formed hetero‐interface weakens the KSe bond of discharged products (K2Se), the length of KSe bond is stretched by 3.9% with an enlargement of 19.2% in angle compared with pure K2Se, greatly promoting the regeneration of MoSe bond during charge. Moreover, the atomically inter‐overlapping feature leads to an expanded MoSe2 interlayer distance of 1.20 nm that enables a much faster K‐ion diffusion. Consequently, this nanoarray delivers an unprecedented K‐ion storage performance, that is, a capacity of 402 mAh g−1 at 0.2 A g−1 over 200 cycles, and a long cycle life over 1000 cycles at 1.0 A g−1 with 307 mAh g−1 capacity retention. [ABSTRACT FROM AUTHOR]

Durable and efficient hydrogen evolution reaction (HER) electrocatalysts that can satisfy industrial requirements need to be developed. Platinum (Pt)‐based catalysts represent the benchmark performance but are less studied for HER under high current densities in neutral electrolytes due to their high cost, poor stability, and extra water dissociation step. Here a facile and low‐temperature synthesis for constructing "blackberry‐shaped" Pt nanocrystals on copper (Cu) foams with low loading as self‐standing electrodes for HER in neutral media is proposed. Optimized hydrogen adsorption free energy and robust interaction induced by charge density exchange between Pt and Cu ensure the efficient and robust HER, especially under high current densities, which are demonstrated from both experimental and theoretical approaches. The electrode exhibits small overpotentials of 35 and 438 mV to reach current densities of ‐10 and ‐1000 mA cm−2, respectively. Meanwhile the electrode illustrates outstanding stability during chronoamperometry measurement under high current densities (‐100 to ‐400 mA cm−2) and 1000 cycles linear sweep voltammetry tests reaching ‐1000 mA cm−2. This study provides new design strategies for self‐standing electrocatalysts by fabricating robust metal–metal interactions between active materials and current collectors, thus facilitating the stable function of electrodes for HER under technologically relevant high current densities. [ABSTRACT FROM AUTHOR]

In this work, a novel low‐cost and thermal conductive composite consisting of boron nitride (BN)/aluminum oxide (Al2O3) heat transfer network was constructed by the high packing volume fraction of two sizes Al2O3 spheres at the optimal weight ratio. The dense packing of 5 μm Al2O3 and 20 μm Al2O3 supports the BN sheets scattering around Al2O3 to interconnect into main three‐dimensional BN network, and acts as thermal conductive bridges forming secondary BN‐Al2O3 heat transfer networks. The maximum thermal conductivity of the composite reached 3.61 Wm−1 K−1, which was 20.1 times more than that of pure epoxy resin. Moreover, the excellent capacity of heat dissipation and the dielectric properties denoted that the composite can be used commendably in electronic components. This article is expected to provide a novel idea for the preparation of economical and high‐performance thermal conductive composites applied in new generation of microelectronic devices. [ABSTRACT FROM AUTHOR]

How to develop an efficient photocatalyst with high activity and high selectivity is the biggest challenge limiting the application of photocatalysis. A reasonable design of the nanoreactor model is an effective strategy. Herein, a series of Pt nanoparticles coated with hexagonal boron nitride (Pt@h‐BN) nanoreactors highly dispersed on a photochemically inert carrier, Al2O3 substrate, are synthesized. The results show that as the number of h‐BN coating layers increases, the selectivity of photocatalysis is altered from nearly 100% CO2‐to‐CO to nearly 100% CO2‐to‐CH4, and the optimized space‐time yield of CH4 is up to 184.7 μmol g(Pt)−1 h−1 with three‐layer coating. The in situ characterizations reveal the cleavage of the CO on Pt to be the rate determining step and the existence of the key intermediate CO2− species on the surface of Pt@h‐BN facilitates CH4 formation. Notably, combined with detailed simulation calculations, this work reveals that the confinement effect in Pt@h‐BN attributes the electrons mobility behavior and alleviate the interaction of COPt. What is more, the change of the reaction site is the essence for the sudden alternation. This work will bring a new insight to the selective catalysis of noble metals in the gas‐solid phase. [ABSTRACT FROM AUTHOR]

The application of polymers in packaging is still limited due to the problems of poor gas barrier and flame retardant properties. Herein, a modified TiO2 (m‐TiO2)@graphene oxide (GO)/montmorillonite (MMT) filler‐reinforced polyvinyl alcohol (PVA)‐based nanocomposite films with excellent gas barrier, flame retardant, and mechanical properties is fabricated through a simple method of solution casting. In this system, GO and MMT act as bricks, PVA sticks them together like glue, and they together form a brick‐wall structure. By adding these fillers, the oxygen permeability rate (Po2) of this film is 0.48 × 10−18 cm3•cm/(cm2•s•Pa), less than that of pure PVA film by 97%, and the water vapor permeability rate (PH2O) of the nanocomposite film is 1.21 × 10−13 g•cm/(cm2•s•Pa), less than that of pure PVA film by 86%. In addition, the flame retardant properties of m‐TiO2@GO/MMT/PVA nanocomposite films are excellent, which self‐extinguishes as long as the flame taken away, different from pure PVA film, which is completely burned. Moreover, the thermal stability and mechanical properties of the nanocomposite films are also significantly improved. The nanocomposites with environment‐friendly raw materials, simple manufacturing processes, and excellent performance should have good applications in the packaging and coating industries. [ABSTRACT FROM AUTHOR]

Mn‐doped 2D perovskites are emerging as good candidates for light‐emitting applications due to their excellent optical and electrical properties. Major synthetic routes, solid‐state grinding and high‐temperature solution synthesis, are extensively studied to prepare Mn‐doped 2D perovskites. However, complicated synthesis, small‐scale yields, and poor‐stability impede their widespread applications. Herein, a one‐step acid‐solution‐assisted method is exhibited for gram‐scale production of Mn‐doped 2D (C8H17NH2)2PbBr4 with a solid yield of 1.35 g products out of 3 mL solvent. After Mn‐doped 2D (C8H17NH2)2PbBr4 being stored in the air for 90 days, the photoluminescence (PL) quantum yield of powders has minor changes, showing good stability. Phosphor‐converted monochrome light‐emitting diodes (LEDs) are fabricated. After the LEDs work 6 h under a voltage of 3 V, their PL spectra have no obvious change, showing a great potential in optoelectronic devices. This study provides a new effective strategy for large‐scale synthesis of ultrastable Mn‐doped 2D perovskites, which is expected to provide inspiration for the industrial optoelectronic applications of perovskites. [ABSTRACT FROM AUTHOR]

Comprehending the characteristics of nanocatalyst and the effect of pretreatment on its catalytic performance is of great importance in the field of catalysis. The present study probes the catalytic performance of fluorinated Pt/Fe2O3 prepared by one step flame spray pyrolysis and the effect of pretreatment in CO oxidation. The characterization reveals that in‐situ fluorination of Pt/Fe2O3 in high temperature flame process contributed to low temperature reducibility, improved dispersion abundant surface oxygen vacancies and reactive hydroxyl groups. It is noteworthy that the optimal catalytic performance was attained after reduction of fluorinated Pt/Fe2O3 in 10% H2 at 200 °C (F‐Pt/Fe‐200). The abundant surface hydroxyl group and oxygen vacancies facilitated faster reaction. The in‐situ DRIFTS reveals the consumption of hydroxyl group in F‐Pt/Fe‐200 which contributed to the amelioration of CO oxidation. Aside the better stability of F‐Pt/Fe‐200, complete conversion of 2% and 4% CO was achieved at 150 °C and 200 °C, respectively, indicating the feasible utilization of flame‐made fluorinated Pt/Fe2O3. Conclusively, the fluorine formed a strong bond with Pt, which ameliorated oxidative and thermal stability. [ABSTRACT FROM AUTHOR]