Vanadium flow batteries (VFBs) are among the most promising technologies for large-scale energy storage due to their high safety, long cycle life, and flexible scalability. However, their deployment in cold climate is hindered by the poor low-temperature stability of vanadium electrolytes. In particular, precipitation of divalent vanadium (V(II)) ions in the negative electrolyte can lead to capacity loss and performance degradation, severely limiting the operating temperature range of VFB systems.Recently, a research team led by Prof. LI Xianfeng from the Dalian Institute of Chemical Physics(DICP), Chinese Academy of Sciences (CAS) uncovered the origin of low-temperature instability in VFB electrolytes and developed a strategy to suppress precipitation through solvation-shell engineering. The study was published in Angewandte Chemie International Edition.By combining single-crystal X-ray diffraction (SCXRD), in situ variable-temperature Raman spectroscopy, and density functional theory (DFT) calculations, the researchers revealed the molecular mechanism of V(II) precipitation. They found that decreasing temperature enhances the dissociation of HSO4-, leading to the accumulation of SO42- ions in solution. These sulfate anions bridge adjacent [V(H2O)6]2+ complexes via hydrogen bonding interaction, promoting V(II) dimerization and the formation of ordered clusters that ultimately evolve into VSO4·xH2O precipitates.Low-temperature instability of the negative electrolyte in VFBs and the corresponding suppression strategy (Image by ZHAN Chengbo and LI Tianyu)To address this issue, the team developed a dual-site solvation engineering strategyby introducing acetonitrile (ACN) and HCl as co-additives to simultaneously regulate the first and second solvation shells of V(II) ions. This synergistic approach effectively suppresses ion aggregation and enhances electrolyte stability at low temperatures.As a result, VFBs employing the modified electrolyte maintained an energy efficiency exceeding 80% over 500 cycles at −10 °C, demonstrating outstanding low-temperature electrochemical performance."Our study provides fundamental insights into the low-temperature behavior of vanadium electrolytes and offers a rational strategy for designing highly stable, wide-temperature-range electrolytes for flow batteries," said Prof. LI.

Cyanohydrins are valuable chemical intermediates used in the production of antidepressants, antiviral drugs, and synthetic plastics. Their conventional synthesis relies on multi-step process involving energy-intensive production of ammonia and hydrogen cyanide, resulting in high energy consumption, high carbon emissions and safety concerns associated with toxic reagents. Developing a direct route to cyanohydrins from abundant feedstock such as nitrogen and methane under mild conditions has long been a major challenge.Schematic illustration of the performance and radical relay mechanism for the reaction of cyclohexanone and non-thermal plasma (NTP)-activated nitrogen and methane (Image by ZHANG Hao)In a study published in Nature Synthesis, a research group led by Profs. DENG Dehui, YU Liang, and HUANG Rui from the Dalian Institute of Chemical Physics (DICP) of the Chinese Academy of Sciences (CAS) developed a plasma-cascade process that enables the direct synthesis of cyclohexanone cyanohydrin [Cy(OH)CN] with nitrogen, methane, and cyclohexanone under mild conditions. The process achieved a Cy(OH)CN selectivity of 95.8% selectivity, a yield of 23.9%, and a formation rate of 0.60 mmol h-1.The researchers proposed a plasma-driven radical cascade mechanism for the reaction. Under non-thermal plasma, nitrogen and methane are excited to generate reactive species, including excited-state nitrogenas well as ·CH3 and ·H radicals, which subsequently react with cyclohexanone.Researchers revealed that plasma-generated ·H radicals first activate the C=O bond of cyclohexanone to form hydroxy-cyclohexyl intermediates, which subsequently undergo C-C coupling with ·CH3 radicals. The resulting α-CHx cyclohexanol species further reacts with excited-state nitrogen to form a C-N bond. Assisted by ·H radicals, the N≡N bond is subsequently cleaved, ultimately yielding the target product cyclohexanone cyanohydrin along with high-value ammonia as a co-product."Our study establishes a new green reaction pathway for the direct one-step synthesis of cyanohydrins from nitrogen and methane with high selectivity, offering a new strategy for the direct and efficient utilization of inert small molecules under mild conditions," said Prof. DENG.

Nonsolvent induced phase separation (NIPS) is a classical method for preparing porous polymeric membranes, which has been widely applied in industrial membrane manufacturing for more than six decades. However, because multiple pore structures form simultaneously during the NIPS process, the underlying microstructure formation mechanism remains incompletely understood. This knowledge gap has hindered the rational design of membrane structures and the precise regulation of membrane performance.In a recent study published in National Science Review, a research team led by Prof. LI Xianfeng from the Dalian Institute of Chemical Physics (DICP) of the Chinese Academy of Sciences (CAS) systematically elucidated the microstructure formation mechanism of NIPS by decoupling the formation of different pores structures, including macrovoids and cellular pores. Based on these findings, the team designed a free-standing ultrathin porous polymeric membrane with a thickness of only 2.7 μm that simultaneously delivers high selectivity and high conductivity. When applied in a vanadium flow battery, the membranes demonstrated outstanding eletrochemical performance.Decoupled formation of macrovoids and cellular pores and the underlying NIPS mechanism (Image by JIA Chaoyang and LU Wenjing)"We developed a novel observation cell for NIPS process, which enabled us to decoupled the formation of macrovoids from that of cellular pores by modulating the flow geometry at the nonsolvent–polymer solution interface," said Prof. LI. Using this experimental setup, the researchers revealed that macrovoid formation originates from hydrodynamic instability and demonstrated that macrovoids growth can be precisely controlled by tuning the interface geometry between the nonsolvent and polymer solution. They further clarified the thermodynamic origin of cellular pores formation and established a quantitative model linking cellular pores area density to key thermodynamic parameters.By eliminating the mass-transfer interference and spatial heterogeneity introduced by macrovoids, the researchers uncovered the intrinsic relationship between membrane formation kinetics and solvent–nonsolvent interdiffusion during the NIPS process. The researchers then investigated the structure–property relationship of porous membranes fabricated through NIPS. Guided by this relationship, they developed a free-standing porous membrane only 2.7 μm thick. When applied in a vanadium flow battery, the membrane achieved an energy efficiency exceeding 80% at a current density of 220 mA/cm2."Our study represents an important advance in the fundamental understanding of NIPS and provides valuable theoretical guidance for the rational design of porous membranes with precisely tunable structures and properties," said Prof. LI.

Ammonia synthesis is a cornerstone of modern agriculture and the chemical industry. It is regarded as a promising carbon-free energy carrier for a future hydrogen economy. However, the performance of conventional transition metal-based catalysts is constrained by the linear scaling relationship (BEP relation), which give rise to a volcano-type activity curve. Early transition metals such as Mn bind N too strongly, making the hydrogenation of activated *N species difficult. As a result, efficient ammonia synthesis catalysts based on early transition metals have rarely been reported.In a recent study published in Angewandte Chemie International Edition, a research team led by Prof. CHEN Ping from the Dalian Institute of Chemical Physics (DICP) of the Chinese Academy of Sciences (CAS), in collaboration with Prof. YUAN Shaojun from Sichuan University, developed an efficient ammonia synthesis catalyst consisting of atomically dispersed early transition metal Mn supported on the ternary hydride (LiBaH3). The catalyst enables efficient ammonia synthesis through a hydride-assisted N2 dissociation mechanism that circumvent traditional scaling relationships.The team synthesized a LiBaH3-Mn1 catalyst, in which the activation of N2 on Mn1 sites, preventing the direct dissociation of N2 to form overly strong Mn-N bonds. Meanwhile, hydride ions (H−) from LiBaH3 further activate the adsorbed *N2 through a reductive protonation pathway, forming *N2H intermediates. Subsequent N–N bond cleavage produces surface nitride (Mn–N) and imide (*NH) species on the LiBaH3–Mn1 interface.The catalyst exhibited an ammonia synthesis rate two orders of magnitude higher than that of manganese nitride and performs 2.5 times better than the benchmark Cs-Ru/MgO catalyst at 400 °C, representing a state-of-the-art performance among group 4–7 transition metal–based catalysts."Our study provides a new strategy for the rational design of highly active early transition metal-based catalysts for ammonia synthesis," said Prof. CHEN.

Recently, in a study published in Angewandte Chemie International Edition, a research team led by Profs. ZHANG Lihua and LIANG Yu from the Dalian Institute of Chemical Physics of the Chinese Academy of Sciences developed a high-throughput strategy for single-cell spatial proteomics boased on an ordered colloidal crystal chromatographic column. This approach improves analytical throughput while maintaining deep proteome coverage, marking a significant advance in single-cell-resolution spatial proteomics.A colloidal crystal chromatographic column assembled from 800 nm monodisperse C18 silica spheres exhibits a tenfold higher column efficiency than conventional sub-2 μm columns, enabling high-throughput spatial proteomics under ultra-short gradients with spatial resolution down to the single-cell level (Image by SUN Haofei and LIANG Yu)Spatial proteomics enables the characterization of protein distribution within biological tissues and plays a critical role in understanding biological functions and disease mechanisms. Single-cell-resolved spatial proteomics is particularly valuable for investigating cellular heterogeneity, signaling pathways, and intercellular interactions within complex tissue microenvironments.Currently, mainstream spatial proteomics relies on nanoLC–MS combined with laser capture microdissection (LCM). However, increasing spatial resolution greatly increases the number of tissue slices, creating a severe throughput bottlenecks. Even with advanced chromatographic columns and high-performance mass spectrometry systems, current single-cell analyses typically require about 30 minutes per sample to achieve sufficient proteome coverage—a major speed constraint for large-scale studies.To address this challenge, the team developed a novel colloidal crystal chromatographic column based on the ordered assembly of 800 nm monodisperse C18 colloidal particles. Benefiting from its highly ordered architecture, submicrometer particle size, and nonporous structure, the column achieved an efficiency exceeding 2 million plates per meter—approximately 10 times higher than that of conventional sub-2 μm chromatographic columns.This substantial improvement enabled dramatically faster proteomic analysis without compromising proteome depth. Using the ordered colloidal crystal column, the team identified 4,462 ± 119 and 3,597 ± 172 proteins from 100 μm-resolution LCM tissue slices under 5-minute and 2-minute separation gradients, respectively. By comparison, conventional sub-2 μm chromatographic columns required a 30-min gradient to achieve similar proteome coverage.When applied to single-cell-resolution spatial proteomics, the method delivered exceptional performance, enabling the identification of up to 2,304 proteins from a single hepatocyte slice within only 5 minutes, while still identifying more than 1,000 proteins under a 2-min gradient.The researchers further applied the method to hepatocellular carcinoma tissues, enabling rapid spatial proteomic characterization of the liver region, early-stage hepatocellular carcinoma, and advanced tumor regions. The approach also revealed proteomic heterogeneity among distinct cell populations within tumor regions at single-cell resolution."Our study provides a high-throughput technological tool for single-cell spatial proteomics, molecular atlas construction, and investigations of disease tissue microenvironments," said Prof. ZHANG.

The selective conversion of methane into high-value oxygenates via C–H activation under mild conditions is considered a promising strategy for energy diversification and greenhouse gas mitigation. In situ generation of H2O2 for methane activation offers an attractive alternative to the use of externally supplied H2O2, avoiding its high cost, low utilization efficiency, and transport and storage risks.However, achieving efficient methane oxidation while suppressing overoxidation remains a major challenge, as it requires precise control over the generation rate, local concentration, and reactive oxygen species derived from H2O2, such as ·OH and ·OOH radicals.In a study published in Angewandte Chemie International Edition, a research team led by Profs. HOU Guangjin and GAO Pan from the Dalian Institute of Chemical Physics (DICP) of the Chinese Academy of Sciences (CAS) developed a Na–Auδ⁻ interface structure on MOR nanosheet that enables near-quantitative selectivity for methane oxidation to methanol, acetic acid, and other oxygenates under mild conditions.Selective methane conversion to methanol and acetic acid via •OH/CH3 radical coupling enabled by Na–Auδ⁻ interfacial sites that generate H2O2 and •OH (Image by Xianquan Li)The researchers found that the Au/1.2Na-MOR(NS) catalyst achieved nearly 100% selectivity toward hydroxylated oxygenates derived from methane, with a productivity of 2.02 mmol·gcat−1·h−1 under CH4/CO/O2/H2O conditions at 150 °C.By combining operando spectroscopic characterizations and density functional theory calculations, the team revealed that the Na–Auδ⁻ interfacial sites promote kinetically favored O–O bond cleavage and H2O dissociation. This process enables the controlled in situ generation of H2O2 and •OH radicals, which are essential for methane C-H activation while effectively suppressing overoxidation.Further mechanistic studies showed that methane oxidation proceeds through *CH3 radicals generated through •OH-mediated methane activation. Coupling of *CH3 with •OH produces methanol, whereas direct coupling with adsorbed CO leads to acetic acid formation. Isotopic labeling experiments confirmed CO serves as the sole carbonyl source, excluding the possibility of methanol carbonylation."Our study elucidates the dynamic role of in-situ generated H2O2 in methane activation under mild conditions and demonstrates that electronic microenvironment engineering is an effective strategy for achieving selective and controllable oxidation valorization of methane," said Prof. HOU.