第16届Angewandte Advances 前沿交叉论坛暨Angewandte Chemie 新刊发布会邀您见证！

Precise catalysis is at the core of breakthroughs in energy and chemical catalysis technologies. It involves precise design and synthesis of catalytic active sites to achieve atomically economical reaction pathways through directional activation of chemical bonds. Our work focuses on the mesoporous carbon supported catalysts tailored for precise catalysis.

Firstly, d/p-electron charge of metal or oxide/sulfide materials which are experimentally measurable are identified as descriptors for catalytic performance. Based on this, principles for designing metal (oxide/sulfide) catalytic materials are proposed, focusing on electronic structure descriptors in catalyst structure-performance relationships. Secondly, utilizing long-range ordered mesoporous structures and local coordination environments, we achieve precise control over electronic structures of active centers, creating mesostructured confined catalysts. Finally, within confined mesospaces, mass transfer and chemical reaction processes can be controlled at the molecular level, and a new mesostructured confined metal precision catalysis system is established with minimal chemical bond transforms, shortest reaction pathways, and lowest carbon emissions.

For example, in the hydrogenation reaction of 2-methyl-3-butyn-2-ol (MBY) to 2-methyl-3-butene-2-ol (MBE), an increase in Pd d-electron charge density changes the adsorption configuration of MBE, breaking the linear scaling relationship. The turn-over frequency (TOF) of Pd/mesoporous carbon catalyst with the highest d charge is 17 times that of Lindlar catalyst, maintaining about 95% MBE selectivity even at close to 100% MBY conversion. A Pd/mesoporous carbon catalyst with increased d charge can simultaneously activate C-H bonds at C2 and C5 positions of pyrrole and thiophene molecules, achieving one-step synthesis of diaryl products with nearly 100% selectivity. This approach shortens reaction steps in traditional homogeneous catalysis.

Environmental and energy-related technologies, including redox flow batteries, fuel cells, water electrolysis, electrochemical carbon capture, and electrodialysis-based ion separation, are pivotal in achieving the dual objectives of peak carbon emissions and carbon neutrality. These technologies rely fundamentally on electromembrane processes, where ion exchange membranes (IEMs) play a critical role by enabling selective ion transport and separating anode and cathode reactions. Traditional IEMs, such as those based on perfluorocarbon Nafion and hydrocarbon polyelectrolytes, are well-established and feature microphase-separated structures. However, they are hindered by the well-known conductivity/selectivity tradeoff, which limits their performance in advanced applications. To address this challenge, our research group has pioneered a new paradigm in membrane design: utilizing confined micropores as ion channels. This innovative approach has been realized through membranes fabricated from charged polymers of intrinsic microporosity, hyper-crosslinked polymers, and ultramicroporous polymer frameworks.The rigidly confined micropores in these next-generation membranes offer a unique combination of high size-exclusion-imposed ion selectivity and high free volume-induced permeability. Remarkably, by leveraging rigid pore confinement and multi-interaction mechanisms between ions and the membrane, triazine framework membranes have achieved near-frictionless ion flow, setting a new benchmark for ion transport efficiency. As next-generation IEMs, these micropore-confined membranes have already demonstrated exceptional performance in organic redox flow batteries and water electrolysis systems. We are confident that their potential extends to a wide range of other electromembrane processes, further advancing the development of sustainable energy technologies. In this presentation, we will provide an overview of traditional IEMs developed in our laboratory and highlight the ground breaking applications of next-generation IEMs in flow batteries and water electrolysis. We will also illustrate how these innovations contribute to the realization of the double carbon goals, paving the way for a cleaner, more sustainable future.

Heterogeneous catalysts play very important roles in many reactions such as hydrogenation, oxidation and energy production. However, it is still challenging for correlating the catalyst structure with their catalytic properties. Atomically precise metal clusters can solve the difficulty, because their total structures can be solved by single-crystal X-ray crystallography. This report is expected to provide a new scientific vision insight into catalytic mechanisms for some reactions on atomically precise metal cluster catalysts, which is completely different from conversional heterogeneous catalysts. Such metal clusters not only provide new opportunities for unraveling catalysis at an atomic level, but also promote the exploration of new chemical processes with metal clusters as well-defined, highly efficient catalysts. It is expected that metal cluster catalysts can ultimately bring metal catalysis to an exciting, new level.

With the development of synthetic chemistry, mesoporous materials have been designed and gradually expanded from single-component to complicated multicomponent structure with richer functions. Simple component mesoporous materials with high surface and adjustable pore architecture have been widely synthesized and developed. Recently, multicomponent mesoporous materials gradually arouse research interest owing to the high-density redox metal sites, variable electronic structures and excellent thermal stability for fulfilling application requirement. However, the exploration for multicomponent MMOs is at early stage and challenging. Our group is committed to the research of synthetic chemistry of multi-component mesoporous materials. Focusing on exploring new chemical synthesis methods, we have achieved the directional preparation of new mesoporous materials, precise modulation of material microstructure and establishment of new methodology by regulating the molecule assembly process as well as the reaction dynamics and thermodynamic equilibrium. The main innovative results achieved are as follows: 1) An interface confined coordination-self-assembly synthetic method was developed, the principle of energy balance was proposed and a series of mesoporous multiple inorganic materials have been synthesized (including perovskite metal oxides, high-entropy metal oxides, polyanionic materials and so on). 2) Synthesis methods of specific polymerization reactions combined with molecule self-assembly were designed and multi-component doped mesoporous carbon materials have been prepared. 3) By discovering new type of template, the solvent-free synthesis methodology for mesoporous materials has been proposed and established, which realize the universal and efficient synthesis for single component and multi-structured mesoporous materials and some achievements have been transformed.

Energy storage systems play a crucial role in the integration of renewable energy sources, which are often unstable and intermittent, such as solar and wind power. These systems ensure a reliable and consistent energy supply by storing excess energy generated during peak production times and releasing it when production is low. Non-aqueous lithium-ion batteries dominate the battery market due to their high energy density, which allows them to store a large amount of energy in a relatively small volume. However, these batteries have a significant drawback: they are flammable. This flammability poses a risk of catastrophic damage, especially in large-scale applications where safety is paramount. Aqueous redox flow batteries (RFBs) offer a promising alternative for scalable, safe, and long-duration energy storage. One of the key advantages of RFBs is their design flexibility, which allows for independent scaling of power and energy capacity. This makes them highly adaptable to various energy storage needs. However, the widespread adoption of all-vanadium redox flow battery is limited by the low abundance and high cost of vanadium, making them less economically viable for large-scale deployment. In this presentation, we will discuss the development of emerging flow battery systems offering low-cost and high-capacity energy storage. We will discuss innovative approaches to mitigate crossover and improve reaction kinetics, thereby making these batteries more efficient and reliable.