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In NH3 capture technologies, the desorption process is usually driven by high temperature and low pressure (such as 150–200 °C under vacuum), which accounts for intensive energy consumption and CO2 emission. Developing light responsive adsorbent is promising in this regard but remains a great challenge. Here, we for the first time designed and synthesized a light responsive azophenol‐containing covalent organic framework (COF), COF‐HNU38, to address this challenge. We found that at 25 °C and 1.0 bar, the cis ‐COF exhibited a NH3 uptake capacity of 7.7 mmol g−1 and a NH3/N2 selectivity of 158. In the adsorbed NH3, about 29.0 % could be removed by vis‐light irradiated cis‐trans isomerization at 25 °C, and the remaining NH3 might be released at 25 °C under vacuum. Almost no decrease in adsorption capacity was observed after eight adsorption‐desorption cycles. As such, an efficient NH3 capture and low energy release strategy was established thanks to the multiple hydrogen bond interactions (which are strong in total but weak in individuals) between NH3 and the smart COF, as well as the increased polarity and number of hydrogen bond sites after the trans‐cis isomerization. [ABSTRACT FROM AUTHOR]

In NH3 capture technologies, the desorption process is usually driven by high temperature and low pressure (such as 150–200 °C under vacuum), which accounts for intensive energy consumption and CO2 emission. Developing light responsive adsorbent is promising in this regard but remains a great challenge. Here, we for the first time designed and synthesized a light responsive azophenol‐containing covalent organic framework (COF), COF‐HNU38, to address this challenge. We found that at 25 °C and 1.0 bar, the cis ‐COF exhibited a NH3 uptake capacity of 7.7 mmol g−1 and a NH3/N2 selectivity of 158. In the adsorbed NH3, about 29.0 % could be removed by vis‐light irradiated cis‐trans isomerization at 25 °C, and the remaining NH3 might be released at 25 °C under vacuum. Almost no decrease in adsorption capacity was observed after eight adsorption‐desorption cycles. As such, an efficient NH3 capture and low energy release strategy was established thanks to the multiple hydrogen bond interactions (which are strong in total but weak in individuals) between NH3 and the smart COF, as well as the increased polarity and number of hydrogen bond sites after the trans‐cis isomerization. [ABSTRACT FROM AUTHOR]

Ionic liquids (ILs) with remarkable performance offer opportunities to advance green and low-carbon chemical processes. Thus, much work is focused on building an innovative theory and knowledge framework to unravel the nature of ILs. Moreover, there is an increasing trend to utilize ILs in rapidly emerging fields. Aiming to provide an overview of the recent advances and challenges of ILs in the development of green processes for renewable resources, this review highlights the properties and functions of ILs in IL gating and as electrolyte additives, modifiers, exfoliation agents, nucleation substrates, tunable solvents, versatile carriers and biosensor components in three representative and revolutionary production processes, namely, new energy, electronic information materials, and biotechnologies. The innovative applications of ILs demonstrate their potential to create a landscape of low-carbon, high-end and smart technologies. [ABSTRACT FROM AUTHOR]

Separating helium (He) and hydrogen (H2), two gases that are extremely similar in molecular size and condensation properties, presents a formidable challenge in the helium industry. The development of membranes capable of precisely differentiating between these gases is crucial for achieving large‐scale, energy‐efficient He/H2 separation. However, the limited selectivity of current membranes has hindered their practical application. In this study, we propose a novel approach to overcome this challenge by engineering submicroporous membranes through the fluorination of partially carbonized hollow fibers. We demonstrate that the fluorine substitution on the inner rim of the micropore walls within the carbon hollow fibers enables tunability of the microporous architecture. Furthermore, it enhances interactions between H2 molecules and the micropore walls through the polarization and hydrogen bonding induced by C−F bonds, resulting in simultaneous improvements in both He/H2 diffusivity and solubility selectivities. The fluorinated HFM‐550‐F‐1 min membrane exhibits exceptional mixed‐gas separation performance, with a binary mixed‐gas He/H2 selectivity of 10.5 and a ternary mixed‐gas He/(H2+CO2) selectivity of 20.8, at 40 bar feed pressure and 35 °C, surpassing all previously reported polymer‐based gas separation membranes, and remarkable plasticization resistance and long‐term continuous stability over 30 days. [ABSTRACT FROM AUTHOR]

Separating helium (He) and hydrogen (H2), two gases that are extremely similar in molecular size and condensation properties, presents a formidable challenge in the helium industry. The development of membranes capable of precisely differentiating between these gases is crucial for achieving large‐scale, energy‐efficient He/H2 separation. However, the limited selectivity of current membranes has hindered their practical application. In this study, we propose a novel approach to overcome this challenge by engineering submicroporous membranes through the fluorination of partially carbonized hollow fibers. We demonstrate that the fluorine substitution on the inner rim of the micropore walls within the carbon hollow fibers enables tunability of the microporous architecture. Furthermore, it enhances interactions between H2 molecules and the micropore walls through the polarization and hydrogen bonding induced by C−F bonds, resulting in simultaneous improvements in both He/H2 diffusivity and solubility selectivities. The fluorinated HFM‐550‐F‐1 min membrane exhibits exceptional mixed‐gas separation performance, with a binary mixed‐gas He/H2 selectivity of 10.5 and a ternary mixed‐gas He/(H2+CO2) selectivity of 20.8, at 40 bar feed pressure and 35 °C, surpassing all previously reported polymer‐based gas separation membranes, and remarkable plasticization resistance and long‐term continuous stability over 30 days. [ABSTRACT FROM AUTHOR]

Dielectric elastomers in the shape of thin films are heavily investigated, but they do not produce beneficial strains and forces comparable to that of skeletal muscles without entailing extremely complicated fabrication processes, rendering their practical use limited. Here, a silicone elastomer fiber is reported that can be produced by the meter and turned into an actuator by a simple process entailing the injection of an ionic liquid as the inner electrode and dipping in an ionogel to form the outer electrode. The fibers range from 174 to 439 µm in outer diameter with wall thicknesses from 62 to 108 µm and can be produced by the meter with regular diameter and thickness. The mechanical properties of the fibers are unaffected by the electrodes and actuation strains of 10% can be achieved, in both dry and wet environments. The fiber actuator can be bundled to mimic human skeletal muscle bundles or used in folded configurations, rendering it ideal as a building block for macroscopic actuators that can be used for many products such as body‐compliant actuators and wearables. [ABSTRACT FROM AUTHOR]

The use of biocompatible ionic liquids (bio-ILs) as a "green" solvent with uniquely tunable cations and anions, specific selectivity, and many other desirable physicochemical properties in biocatalysis has shown great promises to address many challenges. A plethora of studies have demonstrated ILs possess a range of exceptional capabilities in coordinating biocatalysis such as stabilizing enzyme structure, enhancing enzyme-substrate interaction, increasing substrate solubility and product separation/removal, and improving enzyme immobilization/recycling. Therefore, bio-ILs have been explored for biocatalysis in a wide range of homogenous as well as multiphasic systems including biphasic, multiphasic, microemulsion, and whole-cell systems. This review provides an overview of IL-enabled biocatalysis including enzymatic and whole-cell reactions in homogeneous and multiphasic systems. First, the properties of IL concentration, specific ion effect, pH, viscosity, alkyl chain length, hydrophobicity, and polarity on the structures and activities of enzymes are discussed together with characterization techniques to elucidate the mechanisms of IL-enzyme interactions. Second, while homogenous biocatalysis systems containing ILs are briefly introduced and summarized, particular attention is given to multiphasic systems. Furthermore, recent progress in using bio-ILs to modify emerging new enzyme carrier materials including carbonaceous and magnetic nanomaterials, gel microspheres, and membranes as well as their effect on increasing enzyme stability and recycling are highlighted. Finally, we provide our expert opinion for more innovative research in the field and future outlook for the industrial application of ILs in biocatalysis. [ABSTRACT FROM AUTHOR]

Si anode is of paramount importance for advanced energy‐dense lithium‐ion batteries (LIBs). However, the large volume change as well as stress generates during its lithiation‐delithiation process poses a great challenge to the long‐term cycling and hindering its application. Herein this work, a composite binder is prepared with a soft component, guar gum (GG), and a rigid linear polymer, anionic polyacrylamide (APAM). Rich hydroxy, carboxyl, and amide groups on the polymer chains not only enable intermolecular crosslinking to form a web‐like binder, A2G1, but also realize strong chemical binding as well as physical encapsulating to Si particles. The resultant electrode shows limited thickness change of merely 9% on lithiation and almost recovers its original thickness on delithiation. It demonstrates high reversible capacity of 2104.3 mAh g−1 after 100 cycles at a current density of 1800 mA g−1, and in constant capacity (1000 mAh g−1) test, it also shows a long life of 392 cycles. Therefore, this soft‐hard combining web‐like binder illustrates its great potential in the future applications. [ABSTRACT FROM AUTHOR]

Biological CO2 activation and conversion to high-value ethanol are a feasible and green strategy to close the carbon cycle. However, naturally evolved CO2 utilization pathways involve carbon loss or ATP consumption. Herein, we report a complete anabolic pathway for direct conversion of CO2 to ethanol by constructing and assembling three functional modules including CO2 activation, formaldehyde → acetyl-CoA, and ethanol synthesis in a carbon-conserved and ATP-independent system. These artificial ethanol metabolic pathway fluxes were strengthened by screening efficient key enzymes for CO2 activation, promoting formaldehyde assimilation, and employing a two-step reaction. 13C-labeled CO2 demonstrated the feasibility of the pathway converting CO2 into ethanol in vitro by detecting the carbon flow. With this anabolic pathway, we obtained an ethanol concentration of 0.37 mM at a conversion rate of 4.33 nmol CO2 min−1 mg−1 enzyme and 0.5 mM R5P supply. This modularization strategy provides a new avenue in the construction of artificial metabolic pathways for ethanol synthesis from CO2. [ABSTRACT FROM AUTHOR]

Modulating the coordination environment of single‐atom catalysts (SACs) is an attractive approach for maximizing the catalytic activity of single‐atom centers. Currently, the synthesis of low‐coordinated SACs is mainly confined to increasing the pyrolysis temperature (≥900 °C) to control C─N volatile fragments. Herein, a novel and universal strategy for the low‐coordinated SACs modulation is presented using transition metal (e.g., Ni, Co, Zn) ionic liquid precursors under relatively mild temperature of 600 °C, which regulates the L‐shell electronic structure and decreases nearly 50% electrophilic reactivity by ionization of 4‐position N atom, thereby orienting synthesis of the SACs with metal‐N3 centers. The Ni‐N3 SACs exhibit exceptional CO2 electroreduction performance of 99.7% CO Faraday efficiency with an ultra‐high CO partial current density of 467.55 mA·cm−2 as well as a CO production rate up to 10417.51 µmol·h−1·cm−2 in flow cell. The superior catalytic activity achieves over twofold increase compared with the Ni‐N4 SACs prepared by non‐metal ionic liquid precursors due to the lower free energy of the key intermediate *COOH and the stronger adsorption energy. [ABSTRACT FROM AUTHOR]

Ionic liquids (ILs), due to their inherent structural tunability, outstanding miscibility behavior, and excellent electrochemical properties, have attracted significant research attention in the biomedical field. As the application of ILs in biomedicine is a rapidly emerging field, there is still a need for systematic analyses and summaries to further advance their development. This review presents a comprehensive survey on the utilization of ILs in the biomedical field. It specifically emphasizes the diverse structures and properties of ILs with their relevance in various biomedical applications. Subsequently, we summarize the mechanisms of ILs as potential drug candidates, exploring their effects on various organisms ranging from cell membranes to organelles, proteins, and nucleic acids. Furthermore, the application of ILs as extractants and catalysts in pharmaceutical engineering is introduced. In addition, we thoroughly review and analyze the applications of ILs in disease diagnosis and delivery systems. By offering an extensive analysis of recent research, our objective is to inspire new ideas and pathways for the design of innovative biomedical technologies based on ILs. [ABSTRACT FROM AUTHOR]

The development of a sustainable process for producing high-performance photoresists is desirable yet challenging. In this study, we proposed an ionic liquid (IL)-assisted approach for preparing a photoresist by copolymerizing 1-butyl-3-vinyl imidazolium bromide (VBIMBr) and acrylates. The hydrophilic nature of VBIMBr improved the adhesion between the photoresist and the hydrophilic Si substrate, eliminating the use of hazardous hexamethyldisilazane (HMDS) vapor. This IL-based photoresist could be developed with water instead of the corrosive developer tetramethylammonium hydroxide (TMAH). Furthermore, the interaction between VBMIBr and H+ effectively reduced acid diffusion and line edge roughness (LER), resulting in superior lithography performance compared to traditional acrylate photoresists. This IL-based photoresist exhibited an excellent response to both deep ultraviolet lithography (DUV) and electron beam lithography (EBL), achieving a line resolution of 0.5 μm and 100 nm, respectively. Meanwhile, the lithography kinetics and mechanism were further investigated. Overall, this eco-friendly IL-assisted strategy provides a promising solution for producing high-performance photoresists, even in electrical applications. Additionally, this IL-assisted approach has the potential for widespread use in the development of advanced materials. [ABSTRACT FROM AUTHOR]

Ionic liquid-based membranes (ILMs) have garnered significant attention due to the unique coordination properties offered by both ILs and membranes. This makes them a promising area of research with a wide range of potential applications. In recent years, there has been a surge of exciting research activities in the field of ILMs in liquid separation, ranging from fabrication strategies to the development of separation applications. In this review, targeting different types of ILMs, i.e., supported ionic liquid membranes (SILMs), ionic liquid-polymer membranes (ILPMs), poly(ionic liquid) membranes (PILMs), and ionic liquid polymer inclusion membranes (ILPIMs), the preparation strategy, applicability, stability, transport mechanism, and future perspectives are summarized. By providing a comprehensive overview of the different types of ILMs and their applications in liquid separation, this review aims to serve as a valuable resource for researchers and engineers seeking to develop new-type and innovative ILMs for specific separation tasks. It highlights the advantages and limitations of each type of ILMs as well as the various preparation strategies and performance criteria used to evaluate their effectiveness. Ultimately, this information is expected to guide the design and optimization of novel advanced ILMs with enhanced functional properties for real-world applications. [ABSTRACT FROM AUTHOR]

Electrochemical conversion of nitrate to ammonia is an appealing way for small‐scale and decentralized ammonia synthesis and waste nitrate treatment. Currently, strategies to enhance the reaction performance through elaborate catalyst design have been well developed, but it is still of challenge to realize the promotion of reactivity and selectivity at the same time. Instead, a facile method of catalyst modification with ionic liquid to modulate the electrode surface microenvironment that mimic the role of the natural MoFe protein environment is found effective for the simultaneous improvement of NH3 yield rate and Faradaic efficiency (FE) at a low NaNO3 concentration of 500 ppm. Protic ionic liquid (PIL) N‐butylimidazolium bis(trifluoromethylsulfonyl)imide ([Bim]NTf2) modified Co3O4−x is fabricated and affords the NH3 yield rate and FE of 30.23±4.97 mg h−1 mgcat.−1 and 84.74±3.43 % at −1.71 and −1.41 V vs. Ag/AgCl, respectively, outperforming the pristine Co3O4−x. Mechanistic and theoretical studies reveal that the PIL modification facilitates the adsorption and activation of NO3− as well as the NO3−‐to‐NH3 conversion and inhibits hydrogen evolution reaction competition via enhancing the Lewis acidity of the Co center, shuttling protons, and constructing a hydrogen bonded and hydrophobic electrode surface microenvironment. [ABSTRACT FROM AUTHOR]

Electrochemical conversion of nitrate to ammonia is an appealing way for small‐scale and decentralized ammonia synthesis and waste nitrate treatment. Currently, strategies to enhance the reaction performance through elaborate catalyst design have been well developed, but it is still of challenge to realize the promotion of reactivity and selectivity at the same time. Instead, a facile method of catalyst modification with ionic liquid to modulate the electrode surface microenvironment that mimic the role of the natural MoFe protein environment is found effective for the simultaneous improvement of NH3 yield rate and Faradaic efficiency (FE) at a low NaNO3 concentration of 500 ppm. Protic ionic liquid (PIL) N‐butylimidazolium bis(trifluoromethylsulfonyl)imide ([Bim]NTf2) modified Co3O4−x is fabricated and affords the NH3 yield rate and FE of 30.23±4.97 mg h−1 mgcat.−1 and 84.74±3.43 % at −1.71 and −1.41 V vs. Ag/AgCl, respectively, outperforming the pristine Co3O4−x. Mechanistic and theoretical studies reveal that the PIL modification facilitates the adsorption and activation of NO3− as well as the NO3−‐to‐NH3 conversion and inhibits hydrogen evolution reaction competition via enhancing the Lewis acidity of the Co center, shuttling protons, and constructing a hydrogen bonded and hydrophobic electrode surface microenvironment. [ABSTRACT FROM AUTHOR]

As a fuel or energy carrier, hydrogen has been identified as a key way to decarbonize electricity, industry, transportation, and heating sectors. Hydrogen can be produced by a variety of methods, among which water electrolysis driven by renewable energy is sustainable and nearly carbon-free. To use hydrogen widely, storage and transportation over long distances are another key issue. Apart from storage at high pressure and low temperature, hydrogen can be stored in organic compounds via chemical bonding under relatively mild conditions. Efficient utilization of hydrogen includes hydrogen fuel cells as an alternative to internal combustion engines. From the above scenarios, catalysis and reaction media are the key factors for realizing hydrogen energy implementation. Ionic liquids (ILs) offer new opportunities due to their tunable functional groups, low vapor pressure, and stable structures as additives, solvents, and charge transfer materials. ILs are known to produce solid catalysts with controllable properties, decorate solid catalysts with modified electrons and geometric structures, and serve as electrolytes and hydrogen storage media. This review summarizes and recaps the recent progress in how ILs act as a cornerstone to support the production, storage, and utilization of hydrogen. Furthermore, critical challenges and future research directions of ILs in hydrogen energy applications are also outlined. [ABSTRACT FROM AUTHOR]

Coupling Li‐rich Mn‐based oxide (LRMO) cathodes with lithium metal anodes is crucial to enabl high‐energy batteries. However, capacity decline of LRMO caused generally by unexpected parasitic reactions needs to be solved. Herein, an anion synergistic strategy is developed to manipulate the solvation structure to boost the electrochemical performance of high‐voltage lithium batteries. Multi‐salt electrolytes containing TFSI−, DFOB−, and DFBOP− anions are formulated via facilitating a distinctive aggregate, Li+‐(DFBOP−)0.10(DFOB−)0.49(TFSI−)0.51EC0.63EMC2.49DEC0.77, which can reduce the penetration of other anions into the first solvation sheath and strengthen the interaction between Li+ ions and solvent molecules simultaneously. The solvation structure is studied by molecular dynamics (MD) and its feature is found to be able to enhance the transport kinetics of Li+ effectively and favor the formation of an inorganic‐rich interphase. Corrosion of the Al collector is retarded effectively by a cathode−electrolyte interphase (CEI) constructed by the decomposition of DFBOP−, thereby enhancing the cyclability. In addition, Li||LRMO cell can retain its 85% initial capacity after 650 cycles at 1 C. This study provides a guideline to formulate high‐voltage electrolytes with excellent kinetics by regulating the microstructures of solvation and interphases via anion formulation engineering. [ABSTRACT FROM AUTHOR]

Solid electrolytes that can be made compatible with high‐voltage cathodes are greatly desired to increase the energy density of solid lithium metal batteries (SLMBs). However, no monophase polymer or ceramic examples can simultaneously exhibit strong electrochemical stability and reasonable lithium compatibility due to their limited internal energy gap. Herein, a novel asymmetric solid polymer electrolyte (AMSE) with tailored Li+ transport mechanisms is proposed. It is composed of a high‐voltage layer (HVL, polyacrylonitrile/ionic liquid [IL]) and lithium‐compatible layer (LCL, poly(vinylidene fluoride‐co‐hexafluoropropylene)/UiO‐66‐SO3Li). The HVL exhibits a vehicular Li+ transport mechanism with the introduction of IL, which achieves exceptional‐electrochemical stability and reduced interfacial resistance. Due to the complexation between anions and UiO‐66‐SO3Li, a structural diffusion mechanism is achieved in LCL, realizing a quasi‐single‐ion migration in biomimetic ionic channels. The as‐proposed asymmetric configuration, combined with the transport mechanisms, leads to a gradient distribution of electric potential and Li+ in the electrolyte, thus realizing a stable Li+ flux, which is proved by COMSOL‐Multiphysics. The AMSE‐based SLMBs and scale‐up pouch cells show remarkable cycling stability at 4.3 V from room temperature (Li/LiNi0.8Mn0.1Co0.1O2, 3.27 mAh cm−2) to 100 °C. The strategy of facilitating the transport mechanism is expected to provide new pathways for designing next‐generation SLMBs with high energy density. [ABSTRACT FROM AUTHOR]

Mixed matrix membranes (MMMs) are highly promising for natural gas sweetening due to their high microporosity and outstanding gas separation performance. However, MMMs are frequently challenged by the polymer/filler interfacial incompatibility, leading to the deterioration of gas separation performance. In this study, the mixed-linker ZIF-7-8 was employed as a filler by finely tuning the molecular sieving for CO2/CH4 separation. An amino-functionalized ionic liquid ([C3NH2Mim][Cl]) was introduced for constructing the interface connection between the ZIF-7-8 filler and polymer matrix through coordination and hydrogen bonding, which was verified by extended X-ray absorption fine structure (EXAFS) and electron paramagnetic resonance (EPR). The design of interface interaction through an IL is crucial to improve the interface compatibility and the CO2/CH4 separation performance. The newly developed 20% ZIF-7-8-IL (1%)/PI and 25% ZIF-7-8-IL (1%)/PI MMMs displayed a dramatic improvement of CO2 permeability by 244.2% and 291.6%, from 308 to 1060 and 1206 barrer, respectively, for pure-gas separation, compared to the pristine polyimide matrix. Moreover, the 25% ZIF-7-8-IL (1%)/PI MMM also demonstrated outstanding low-temperature mixed-gas CO2/CH4 separation performance in the temperature range of −45–35 °C, far beyond the 2018 mixed-gas CO2/CH4 upper bound. [ABSTRACT FROM AUTHOR]

The separation of rare earth elements is particularly difficult due to their similar physicochemical properties. Based on the tiny differences of ionic radius, solvent extraction has been developed as the "mass method" in industry with hundreds of stages, extremely intensive chemical consumption and large capital investments. The differences of the ionic magnetic moment among rare earths are greater than that of ionic radius. Herein, a novel method based on the large ionic magnetic moment differences of rare earth elements was proposed to promote the separation efficiency. Rare earths were firstly dissolved in the ionic liquid, then the ordering degree of them was improved with the Z-bond effect, and finally the magnetic moment differences between paramagnetic and diamagnetic rare earths in quasi-liquid system were enhanced. Taking the separation of Er/Y, Ho/Y and Er/Ho as examples, the results showed that Er(III) and Ho(III) containing ionic liquids had obvious magnetic response, while ionic liquids containing Y(III) had no response. The separation factors of Er/Y and Ho/Y were achieved at 9.0 and 28.82, respectively. Magnetic separation via quasiliquid system strategy provides a possibility of the novel, green, and efficient method for rare earth separation. [ABSTRACT FROM AUTHOR]

The key to realize long‐life high energy density lithium batteries is to exploit functional electrolytes capable of stabilizing both high voltage cathode and lithium anode. The emergence of localized high‐concentration electrolytes (LHCEs) shows great promise for ameliorating the above‐mentioned interfacial issues. In this work, a lithium difluoro(oxalate)borate (LiDFOB) based nonflammable dual‐anion LHCE is designed and prepared. Dissolving in the mixture of trimethyl phosphate (TMP) /1,1,2,2‐tetrafluoroethyl‐2,2,3,3‐tetrafluoropropylether (D2), the continuously consumption of LiDFOB is suppressed by simply introducing lithium nitrate (LiNO3). Meantime, as most of the TMP molecular are coordinated with Li+, the electrolyte does not show incompatibility issue between neither metal lithium nor graphite anode. Therefore, it demonstrates excellent capability in stabilizing the interface of Ni‐rich cathode and regulating lithium deposition morphology. The Li||LiNi0.87Co0.08Mn0.05O2 (NCM87) batteries exhibit high capacity retention of more than 90% after 200 cycles even under the high cutoff voltage of 4.5 V, 1 C rate. This study offers a prospective method to develop safe electrolytes suitable for high voltage applications, thus providing higher energy densities. [ABSTRACT FROM AUTHOR]

Rechargeable aluminum ion batteries (AIBs) are one of the most promising battery technologies for future large‐scale energy storage due to their high theoretical volumetric capacity, low‐cost, and high safety. However, the low capacity of the intercalation‐type cathode materials reduces the competitiveness of AIBs in practical applications. Herein, a conversion‐type FeF3‐expanded graphite (EG) composite is synthesized as a novel cathode material for AIBs with good conductivity and cycle stability. Combined with the introduction of a single‐wall carbon nanotube modified separator, the shuttle effect of the intermediate product, FeCl2, is significantly restrained. Moreover, enhanced coulombic efficiency and reversible capacity are achieved. The AIB exhibits a satisfying reversible specific capacity of 266 mAh g−1 at 60 mA g−1 after 200 cycles, and good Coulombic efficiency of nearly 100% after 400 cycles at a current density of 100 mA g−1. Ex situ X‐ray diffraction and X‐ray photoelectron spectroscopy are applied to explore the energy storage mechanism of FeF3 in AIBs. The results reveal that the intercalation of Al3+ species and the reduction of Fe3+ species occurrs in the discharge process. These findings are meaningful for the fundamental understanding of the FeF3 cathode for AIBs and provide unprecedented insight into novel conversion type cathode materials for AIBs. [ABSTRACT FROM AUTHOR]

Bilayer graphene (BLG) is gaining increasing attention as one of the most promising candidate materials for post-silicon nanoelectronics. It is still a tremendous challenge to selectively and efficiently produce BLG at low cost and under mild conditions. Herein, a novel strategy of bilayer-favored intercalation (BFI) induced liquid phase exfoliation of BLG under mild conditions was developed. This simple approach can effectively exfoliate graphite to give BLG with a high yield of 52.3%, and selectivity as high as 86.5%. The obtained twisted BLG not only maintains the structural integrity and low surface oxidation of graphene, but also demonstrates great electron mobility. With careful experimental design and use of DFT calculations, such efficient production of BLG is proved to originate from the formation of a stage-two graphite intercalation compound via the bilayer-favored intercalation of chromyl chloride (CrO2Cl2) into graphite flakes driven by the electrostatic interactions between CrO2Cl2 and graphene sheets. The BFI-induced liquid phase exfoliation strategy shows great potential for the industrial scale production of high-quality BLG. [ABSTRACT FROM AUTHOR]

Supercapacitors (SCs) are fascinating energy storage devices due to their delivery of exceptional power density and long cycling stability. Unfortunately, their practical applications are still impeded by relatively inferior energy density, which is proportional to the square of the operating voltage of SCs. Ionic liquid (IL) electrolytes have a wide electrochemical stability window and thus can be used to significantly increase the energy density of SCs. The introduction of redox active species into IL‐based electrolytes effectively contributes to pseudocapacitance. Accordingly, IL‐based redox active electrolytes (IL‐REs) for SCs are springing up rapidly in recent years. This review provides an overall insight into various IL‐REs, including the ILs mixed with other redox active species, the ILs possessing redox active groups themselves, and the IL‐based redox gel polymer electrolytes for SCs. The basic understanding of IL electrolytes and IL‐REs is introduced and discussed as well as the application of the IL‐REs in SCs. Then, the energy storage mechanisms of these IL‐REs are discussed, and finally, current challenges and perspectives are highlighted for future research in this promising field. [ABSTRACT FROM AUTHOR]

Understanding the ionic transport behaviors in hybrid solid electrolytes (HSEs) is critically important for the practical realization of rechargeable Li‐metal batteries (LMBs) with high safety. Herein, it is reported a new solid "Ionogel‐in‐Ceramic" electrolyte by using the Li1.3Al0.3Ti1.7(PO4)3 (LATP) ceramic particles as a framework and "Poly(ionic liquid)s‐in‐Salt" ("PolyIL‐in‐Salt") ionogel as an ionic bridge via a simple pressing process. The "PolyIL‐in‐Salt" ionogel precursor is designed to improve the chemical compatibility at solid–solid interfaces. Molecular dynamics simulations reveal the roles of salt concentrations on the distribution of co‐coordination of "PolyIL‐in‐Salt" ionogel. Moreover, the "PolyIL‐in‐Salt" ionogel containing co‐coordination not only inhibits the parasitic reactions between LATP and Li anode but also provides efficient Li+ conducting pathways. Benefiting from the designed structure, the "Ionogel‐in‐Ceramic" HSE exhibits an excellent ionic conductivity of 0.17 mS cm−1 at 50 °C. Meanwhile, the as‐formed solid electrolyte enables a long cycle of over 3500 h in Li/Li symmetric cell. Further, all‐solid‐state lithium metal batteries fabricated on LiFePO4 and high voltage LiCoO2 cathodes deliver 160.0 mAh g−1, 125.0 mAh g−1, respectively. This study sheds light on the rational design of solid‐state electrolytes with efficient interparticle Li+ conduction, compatible, stable, compact, and durable electrode–electrolyte interfaces. [ABSTRACT FROM AUTHOR]

The enormous emission of carbon dioxide (CO2) from industries has triggered a series of environmental issues. In recent years, ionic liquids (ILs) as novel absorbents are widely used for CO2 capture owing to their low vapor pressure and tunable structures. IL‐modified adsorbents have the advantages of both ILs and porous supports, such as high CO2 selectivity and high specific surface area, which are novel agents to capture CO2 with broad application prospects. In this review, more than 140 IL‐modified adsorbents for CO2 capture in recent years were systematically summarized. The types of ILs including conventional ILs and functionalized ILs on CO2 separation performance of different IL hybrid adsorbents, and their adsorption mechanisms were also discussed. Finally, future perspectives on IL‐modified adsorbents for CO2 separation were further posed. [ABSTRACT FROM AUTHOR]

Summary: Catalytic effects in fast pyrolysis of low‐rank coal and coal tar conversion were investigated in a two‐stage fixed‐bed reactor over HZSM‐5 zeolite and Mg/HZSM‐5. Mg/HZSM‐5 caused the lower total tar yield and the higher non‐condensable gas yield but the fraction of light tar (boiling point below 360°C) increased to allow a slightly higher total yield of light tar. It also exhibited good catalytic activity and increased the species of light tar than HZSM‐5 zeolite. The light tar fraction was increased from 45 to 74.6 wt% than without catalyst (66%) at the pyrolysis temperature of 600°C. Ex‐situ catalytic fast pyrolysis over Mg/HZSM‐5 also lowered the contents of element N and S in the resulting coal tars by 29% and 15% respectively. The corresponding increase in the content of element H and molar ratio of H to C of the resulting coal tars was reported as 17% and 13% respectively. The addition of Mg into HZSM‐5 increased the ability of the catalyst for inhibiting coke deposition. [ABSTRACT FROM AUTHOR]

Ionic liquids and deep eutectic solvents are of growing interest as solvents for the resource‐efficient synthesis of inorganic materials. This Review covers chemical reactions of various deep eutectic solvents and types of ionic liquids, including metal‐containing ionic liquids, [BF4]−‐ or [PF6]−‐based ionic liquids, basic ionic liquids, and chalcogen‐containing ionic liquids. Cases in which cations, anions, or both are incorporated into the final products are also included. The purpose of this Review is to raise caution about the chemical reactivity of ionic liquids and deep eutectic solvents and to establish a guide for their proper use. [ABSTRACT FROM AUTHOR]

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Nylon is a polyamide material with excellent performance used widely in the aviation and automobile industries, and other fields. Nylon monomers such as hexamethylene diamine and other monomers are in huge demand. Therefore, in order to expand the methods of nylon production, we tried to develop alternative bio‐manufacturing processes which would make a positive contribution to the nylon industry. In this study, the engineered E. coli‐overexpressing Lysine decarboxylases (LDCs) were used for the bioconversion of l‐lysine to cadaverine. An integrated fermentation and microfiltration (MF) process for high‐level cadaverine production by E. coli was established. Concentration was increased from 87 to 263.6 g/L cadaverine after six batch coupling with a productivity of 3.65 g/L‐h. The cadaverine concentration was also increased significantly from 0.43 g cadaverine/g l‐lysine to 0.88 g cadaverine/g l‐lysine by repeated batch fermentation. These experimental results indicate that coupling the fermentation and membrane separation process could benefit the continuous production of cadaverine at high levels. [ABSTRACT FROM AUTHOR]

The efficient bioactivation of CO2 provides an alternative new strategy for producing high value chemicals and fuels. Normally, in vitro activation of CO2 can be achieved by using formate dehydrogenase (FDH). However, the CO2 solubility and the activity of commercial FDHCb remain a tough challenge for the efficient bioactivation of CO2. Here, we report a new "ionozyme" strategy created by using ionic liquids (ILs) as a solvent and enzyme stabilizer, resulting in a 142.3-fold increase in CO2 conversion over FDHCb. The ionozyme (FDHPa-[CH][Pro]-[TMGH][PhO]) was first developed by combing a discovered novel FDHPa with an efficient synergistic ionic microenvironment. The remarkable performance of this ionozyme is attributed to forming key intermediates [CH][ProCOO] and [TMGH][PhOCOO], stabilizing the enzyme structure with increased solvation structure, and shortening the distance (3.9 Å) between NADH and CO2 to favor the hydride transfer by facilitating their relative orientation and forming new hydrogen bonds at the active sites. This bioactivation of CO2 by this specific ionozyme represents ideal starting points for the sustainable carbon cycle. [ABSTRACT FROM AUTHOR]

The high cost and limited supply of platinum has driven intensive research into the use of non-platinum group metals (PGM-free) as cathode oxygen reduction reaction (ORR) catalysts for proton exchange membrane fuel cells (PEMFCs), which is crucial in promoting the large-scale applications of PEMFCs and the most important step to achieve the DOE ultimate stack cost target. As the most promising group of PGM-free ORR catalysts, the metal/N/C (M–N–C) catalysts have been extensively explored. However, several problems still exist in the development of high-performance M/N/C catalysts, including limited intrinsic activity and durability, severe concentration polarization and ohmic polarization. Therefore, our aim is to conduct a comprehensive understanding and recognize the strengths and weaknesses of the state-of-the-art PGM-free ORR catalysts for PEMFCs. Herein, we summarize three classes of the most active M/N/C ORR catalysts, namely, conductive PANI-based catalysts and their analogues, ZIFs-based catalysts and their derivatives, and other high-performance ORR catalysts, thoroughly expound their deactivation mechanisms, and deeply discuss the oxygen reduction mechanisms and approaches for identifying active sites. The challenges and perspectives on PGM-free cathode catalysts of PEMFCs are also discussed. [ABSTRACT FROM AUTHOR]

Developing solid‐state electrolytes with good compatibility for high‐voltage cathodes and reliable operation of batteries over a wide‐temperature‐range are two bottleneck requirements for practical applications of solid‐state metal batteries (SSMBs). Here, an in situ quasi solid‐state poly‐ether electrolyte (SPEE) with a nano‐hierarchical design is reported. A solid‐eutectic electrolyte is employed on the cathode surface to achieve highly‐stable performance in thermodynamic and electrochemical aspects. This performance is mainly due to an improved compatibility in the electrode/electrolyte interface by nano‐hierarchical SPEE and a reinforced interface stability, resulting in superb‐cyclic stability in Li||Li symmetric batteries (>4000 h at 1 mA cm−2/1 mAh cm−2; >2000 h at 1 mA cm−2/4 mAh cm−2), which are the same for Na, K, and Zn batteries. The SPEE enables outstanding cycle‐stability for wide‐temperature operation (15–100 °C) and 4 V‐above batteries (Li||LiCoO2 and Li||LiNi0.8Co0.1Mn0.1O2). The work paves the way for development of practical SSMBs that meet the demands for wide‐temperature applicability, high‐energy density, long lifespan, and mass production. [ABSTRACT FROM AUTHOR]

Nano-porous electrodes combined with ionic liquids (ILs) are widely favored to promote the energy density of supercapacitors. However, this is always accompanied by the reduced power density, especially considering the high viscosity and large steric hindrance of ILs. Here, we use computational simulations coupled with the equivalent circuit model to quantify the charging process and overall performance of the IL-based supercapacitor. We find that the ions in the electrode with ionophobic pores display a new charging mechanism under a threshold potential, namely co-ion adsorption, which has been ignored before. This identified abnormal charging process can not only efficiently enhance the differential capacitance but also remarkably speed up the charging dynamics. Meanwhile, the pores with various sizes and lengths in the electrode demonstrate the same tendency, reflecting the relative universality of the collaborative enhancement of the co-ion adsorption process. Furthermore, the quantitative relation between charging time/capacitance and electric voltage/ionophobic properties is further obtained to evaluate the critical conditions for synergistically improving the energy density and power density of supercapacitors. These findings may advance the understanding of charging mechanisms in porous electrodes and manifest that the ionophobicity is one important factor in the rational design of supercapacitors with ILs or other electrochemical devices in the field of chemical engineering. [ABSTRACT FROM AUTHOR]

A Cu–N-doped carbon nanotube with an unsaturated coordination Cu atom (Cu–N3) was fabricated and it exhibited over 90% CO faradaic efficiency (FE) in a wide potential range from −0.42 to −0.92 V. The maximum CO FE can reach 98.7% with a high CO partial current density of 234.3 mA cm−2 in a flow cell. Theoretical calculations elucidated that the Cu–N3 site facilitated the formation of COOH*, thereby accelerating the CO2 electrochemical reduction. [ABSTRACT FROM AUTHOR]

Direct cleavage of the C–C bond in lignin linkages is a promising route to afford value-added aromatics, which, however, usually involves metal-based catalysts and harsh conditions. Here, a photo-thermal strategy is reported to deconstruct the Cα–Cβ bond in lignin β-O-4 and β-1 interlinkages in the ionic liquid [BMim][NTf2]. It was found that the synergism of UV light and heating could trigger the Norrish type I reaction by inducing the cleavage of the Cα–Cβ bond and afford aromatic aldehydes through a free radical route in modest yields. Meanwhile, [BMim][NTf2] could interact with lignin moieties and stabilize the intermediates, which significantly contribute to the Cα–OH protonation and accelerate lignin interunit linkage breakage. In this unique route, the Cα–Cβ bond could be cleaved at 50 °C under UV light irradiation without the presence of a metal. Further comparison with photochemical or thermochemical alone strategies demonstrates that the photo-thermal route offers a significant improvement in the Cα–Cβ bond cleavage reactivity. Alkali lignin could also be degraded into aromatic monomers in [BMim][NTf2] using the protocol. Given the necessity of biomass upgradation, this work may provide a green and unique technology to boost the inert C–C bond cleavage upon photo-thermal synergism under metal-free and mild conditions that may underpin future advances in photo-thermal transformation and renewable energy production. [ABSTRACT FROM AUTHOR]

In order to overcome the disadvantages of excessive water and many byproducts in the conventional process of epoxide hydration into 1,2-diols, 2-carboxylated imidazolium salts were first adopted as efficient catalysts for one-step hydration of epoxides into 1,2-diols. By regulating the cation chain lengths, different steric structures of 2-carboxylated imidazolium salts with chain lengths from C1 to C4 were prepared. The salt with the shortest substituent chain (DMIC) exhibited better thermal stability and catalytic performance for hydration, achieving nearly 100% ethylene oxide (EO) conversion and 100% ethylene glycol (EG) selectivity at 120 °C, 0.5 h with just 5 times molar ratio of H2O to EO. Such a tendency is further confirmed and explained by both XPS analysis and DFT calculations. Compared with other salts with longer chains, DMIC has stronger interaction of CO2− anions and imidazolium cations, exhibiting a lower tendency to release CO2− and form HO–CO2−, which can nucleophilically attack and synergistically activate ring-opening of epoxides with imidazolium cations. The strong huge sterically dynamic structure ring-opening transition state slows down the side reaction, and both cations and anions stabilized the transition state imidazolium-EG-HO–CO2−, both of which could avoid excessive hydration into byproducts, explaining the high 1,2-diol yield. Based on this, the cation–anion synergistic mechanism is then proposed. [ABSTRACT FROM AUTHOR]