Xiu-Liang Lv

Chat-RFB integrates knowledge graphs with large language models to enable accurate, source-verified scientific dialogue and accelerate discovery in redox flow battery research.

This review establishes molecule-to-system design rules that connect TEMPO/viologen molecular engineering with neutral-pH battery assembly and grid-scale deployment, emphasizing cost, safety, and scalability.

The interdisciplinary nature of redox flow batteries (RFBs), spanning chemistry, materials, and engineering, has led to a vast and fragmented body of research, hindering the efficient synthesis of knowledge. An intelligent question-answering system is there-fore essential to organize this dispersed knowledge, enhance information retrieval, and lower the barrier to comprehensive understanding. In this study, we leveraged the natu-ral language processing capabilities of large language models (LLMs) and the structured nature of knowledge graphs (KGs) to establish a chat model in the field of RFB, named Chat-RFB. By analyzing 5,353 articles related to flow batteries and deconstructing the text content, we learned contextual relationships and generated nearly 164,232 nodes, constructing 853,939 relationships among nodes. This process enhances the profession-al domain knowledge question-answering ability of LLMs. Given the limited research on the responsiveness of evaluation models in the flow battery field, we conducted model performance evaluations using both choice and non-choice questions. The results indicate that by incorporating a professional knowledge base, Chat-RFB enhanced the level of professional domain knowledge. Choice question accuracy was: Chat-RFB 94.9%, DeepSeek-v3 90.9%, GPT-4o 90.7%, Qwen-Max 90.4%, Gemini-2.5-Flash 91.1%. Non-choice question accuracy was: Chat-RFB 93.3%, DeepSeek-v3 75.6%, GPT-4o 68.9%, Qwen-Max 73.3%, Gemini-2.5-Flash 86.7%.

We present a two-dimensional (2D) electrically conductive metal-organic framework (EC-MOF)-based artificial synapse. The intrinsic electronic conductivity and subnanometer channels of the EC-MOF facilitate efficient ion diffusion, enable a high density of active redox centers, and significantly enhance capacitance within the artificial synapse. As a result, the synapse operates at an ultralow voltage of 10 mV and exhibits a remarkably low power consumption of approximately 1 fW, along with the longest retention time recorded for two-terminal electrolyte-type artificial synapses to date. The alignment of the quantum size of the subnanometer pores in the EC-MOF with various cations allows for versatile synaptic plasticity. This capability is applied to image refresh, classification, and efferent signal transmission for controlling artificial muscles, thereby offering a methodology for achieving tunable neuromorphic properties. These findings suggest the potential application of metal-organic frameworks in artificial nervous systems for future brain-inspired computation, peripheral interfaces, and neurorobotics.

Aqueous redox flow batteries with halide-based catholytes (where the halogen atom (X) is Br or I) are promising for sustainable grid energy storage. However, the formation of polyhalides during electrochemical charging and the associated phase separation into X₂ limits the operable state of charge (SoC), results in vaporization and self-discharge inefficiencies, and spurs complete device failure^1,2,3. Here we introduce soft–hard zwitterionic trappers (SH-ZITs) as complexing agents composed of a polyhalide-complexing ‘soft’ cationic motif and a water-soluble ‘hard’ anionic motif to enable homogeneous halide cycling. More than 300 structures were designed and 13 were characterized, showcasing the ability to complex polyhalides in homogeneous aqueous solution, to deter cation-exchange membrane crossover and to alter the electrochemical electrode mechanism. In flow battery cycling at a standard catholyte SoC of 66.6 per cent (stoichiometrically X₃^–), an average coulombic efficiency of more than 99.9 per cent at 40 milliamperes per square centimetre with no apparent decay was observed after more than 1,000 cycles over 2 months, with stability at elevated temperatures also demonstrated. Interestingly, SH-ZITs enable homogeneous cycling of the halide catholyte up to 90 per cent SoC at 2 moles per litre (47.7 ampere-hours per litre) for bromide, revealing previously unknown polyhalide regimes to be studied. Ultimately, SH-ZIT enables ultrahigh catholyte capacity utilization up to over 120 ampere-hours per litre at 80 per cent SoC with homogeneous cycling as well as the ability to pair with a zinc anode in a hybrid flow battery.

Due to the unique photophysical and electrochemical properties of porphyrins, porphyrin-based metal–organic frameworks (PMOFs) offer an excellent platform for heterogeneous catalysis applications and the fundamental study of structure–property relationships based on their crystalline nature. In this study, we investigate the impact of porphyrin ligands with different substituents on the structural diversity of derived Zr(IV)-based PMOFs (Zr-PMOFs), with a particular emphasis on the advantage of a bifunctional pyridyl-carboxylate porphyrinic ligand in tuning the structure and catalysis performance of resultant PMOFs. Two highly stable and porous Zr-PMOFs (BUT-229 and -230) prepared from the bifunctional porphyrinic ligand have similar constituents but different structural topology due to their ligands adopting different conformations. Noteworthily, the catalytic performance of Zr-PMOFs could be profoundly affected by the conformation of their porphyrinic ligands, which determines not only the topology, porosity, and catalytically active center density of the PMOFs, but also their photoelectric properties, including visible-light absorption, bandgap, electron transfer and charge separation efficiency. As a rare example of PMOFs with the flu topology, BUT-229 afforded obviously higher catalytic activity than BUT-230 as well as some benchmark PMOFs in the photo-oxidation reaction of benzyl alcohol. Moreover, with Lewis base sites (free pyridyl N atoms) on pore surfaces, BUT-229 could efficiently catalyze the tandem reactions between aromatic alcohols and active methylene compounds under mild conditions. Its catalytic activity was further enhanced by partially appending covalently the cocatalyst TEMPO (TEMPO = 2,2,6,6-tetramethylpiperidinooxy) to the free pyridyl groups via the Zincke reaction. These results provide insights into the development of high-performance porphyrin-based catalysts for tandem organic reactions.

Further development of metal–organic frameworks (MOFs) requires an establishment of hierarchical interaction within the framework. Herein, we report a series of mesoporous rare‐earth (RE) MOFs that are constructed from an unusual 12‐connected π‐stacked pyrene secondary building unit (SBU) and a typical 12‐connected RE₆ cluster (RE=Eu, Y, Yb, Tb, Ce). The judicious design of a butterfly‐shape pyrene ligand with a tert‐butyl substituent enables the formation of the disordered 12‐connected organic SBUs on its strong intermolecular π–π interactions. The assembly of 12‐connected inorganic cuboctahedron SBUs and 12‐connected organic distorted hexagonal prism SBUs generates an unprecedented network that can be further simplified into a 4,4‐connected pts net linked from planar square and tetrahedra. This work provides fresh insights into the design and synthesis of frameworks constructed from coordinatively, covalently, and noncovalently linked building units.