Bo Zhang

The high‐efficiency electrosynthesis of hydrogen peroxide (H ₂ O ₂ ) via two‐electron oxygen reduction reaction (2e ⁻ ORR) represents a promising alternative to the traditional anthraquinone process. However, achieving high selectivity, industrial‐grade stability, and on‐site utilization of H ₂ O ₂ remains a significant challenge. Here, we designed a single‐atom catalyst, CoNPC, featuring a Co–N/P co‐coordination structure, tailored for high‐current‐density H ₂ O ₂ electrosynthesis and relevant paired valorization of ethylene glycol. The P modulation optimized the electronic structure of Co centers, leading to enhanced selectivity (> 90%) and stable H ₂ O ₂ production for over 140 h at a high current density of −200 mA cm ⁻² . In situ spectroscopic studies and theoretical calculations revealed that the P heteroatom plays a critical role in optimizing *OOH binding energy, thereby facilitating the 2e ⁻ ORR process. The electrogenerated H ₂ O ₂ was further utilized in a Fenton‐like process to oxidize ethylene glycol to formic acid. By coupling this cathodic reaction with anodic EG electrooxidation, we demonstrated a paired electrolysis system that enables simultaneous value‐added products at both sides. This work not only offers a robust strategy for the design of single‐atom catalysts on industrial H ₂ O ₂ electrosynthesis but also pioneers an energy‐efficient paired electrolysis system for waste utilization.

The high‐efficiency electrosynthesis of hydrogen peroxide (H ₂ O ₂ ) via two‐electron oxygen reduction reaction (2e ⁻ ORR) represents a promising alternative to the traditional anthraquinone process. However, achieving high selectivity, industrial‐grade stability, and on‐site utilization of H ₂ O ₂ remains a significant challenge. Here, we designed a single‐atom catalyst, CoNPC, featuring a Co–N/P co‐coordination structure, tailored for high‐current‐density H ₂ O ₂ electrosynthesis and relevant paired valorization of ethylene glycol. The P modulation optimized the electronic structure of Co centers, leading to enhanced selectivity (> 90%) and stable H ₂ O ₂ production for over 140 h at a high current density of −200 mA cm ⁻² . In situ spectroscopic studies and theoretical calculations revealed that the P heteroatom plays a critical role in optimizing *OOH binding energy, thereby facilitating the 2e ⁻ ORR process. The electrogenerated H ₂ O ₂ was further utilized in a Fenton‐like process to oxidize ethylene glycol to formic acid. By coupling this cathodic reaction with anodic EG electrooxidation, we demonstrated a paired electrolysis system that enables simultaneous value‐added products at both sides. This work not only offers a robust strategy for the design of single‐atom catalysts on industrial H ₂ O ₂ electrosynthesis but also pioneers an energy‐efficient paired electrolysis system for waste utilization.

The dielectric response of carbon‐based single‐atom (SA) absorbers is intrinsically constrained by the highly symmetric charge distribution of planar M‐N ₄ coordination motifs, which suppresses dipole polarization and limits electromagnetic wave (EMW) attenuation. Here, a nanocurvature‐driven symmetry‐breaking strategy is proposed to activate latent dielectric polarization at SA sites through geometric regulation. By combining click chemistry with template‐assisted synthesis, metal SAs are anchored onto hollow nitrogen‐doped carbon spheres with precisely tunable diameters, enabling systematic modulation of local nanocurvature. Theoretical calculations and experimental analyses reveal that curvature‐induced surface charge accumulation disrupts the electronic symmetry at Ni‐N ₄ centers, markedly enhancing local charge density, dipole moments, and polarizability. Consequently, the optimized Ni/HNC‐200 absorber achieves an ultralow minimum reflection loss of −74.1 dB, representing a staggering 390% enhancement over HNC‐200 (−15.1 dB), and exhibits a reduced radar cross section of −70.49 dB m ² . A flexible electronic patch further demonstrates over fivefold suppression of electric‐field radiation from mobile phone chips. The universality of this mechanism is validated in Co‐ and Cu‐based systems, establishing nanocurvature as a geometry‐enabled design paradigm for high‐performance SAs EMW absorbers.

Lignocellulose offers a high potential for replacing fossil fuels. Its primary components—cellulose, hemicellulose, and lignin—can be catalytically transformed into value-added chemicals. The involvement of nitrogen in the degradation of lignocellulose to produce bio-based nitrogen (N)-containing compounds is emerging as a key research focus. This research area is very important because it not only transcends the conventional limitations of C/H/O-containing compounds production but also offers substantial theoretical and practical insights into the rational utilization of lignocellulosic feedstocks. Therefore, with this review we provide insights into accomplishments for the transformation of major components of lignocellulosic biomass, including polysaccharide-derived platform compounds, lignin model compounds, lignin and lignocellulose feedstocks, into value-added N-containing compounds. The focus is on analyzing catalytic systems and reaction mechanisms involving C–O/C–C bond cleavage, as well as C–N bond formation. An outlook is offered to outline the key challenges and future perspectives in this rapidly growing field.

Well-defined single-atom catalysts (SACs) serve as ideal model systems for directly comparing experimental results with theoretical calculations, offering profound insights into heterogeneous catalytic processes. However, precisely designing and controllably synthesizing SACs remain challenging due to the unpredictable structure evolution of active sites and generation of embedded active sites, which may bring about steric hindrance during chemical reactions. Herein, we present the precious nonpyrolysis synthesis of Re SACs with a well-defined phenanthroline coordination supported by NiO (Re₁-phen/NiO). Multiple experimental characterizations together with theoretical calculations unravel the idea that the isolated Re atoms are suspended on the NiO surface, connected by phenanthroline ligands standing perpendicular to the surface. This unique structure provides the Re₁-phen/NiO SAC with a strong capability to activate glucose molecules, enabling fully exposed Re=O double bonds in an open-ended reaction environment to simultaneously react with hydroxyl and aldehyde groups at both ends of the glucose molecule, rapidly forming glucaric acid.

We have constructed a series of model metal phthalocyanines (MPc) for the carbon dioxide reduction reaction (CO₂RR), constructed a volcano relationship through density functional theory (DFT) and experiments, and obtained cobalt phthalocyanine (CoPc) at the apex. The volcano diagram is conducive to the screening of catalysts and has a guiding role in the design of catalysts.

生物质作为一种重要的可再生资源, 因其含有丰富的碳、氢、氧元素和环境友好的特性, 是可能替代化石能源的主要可再生能源之一. 目前, 生物质资源可通过高值化转化制备生物基化学品、材料和燃料等, 其中, 含氮化合物是一类重要的有机含氮化学品, 在医药、农业和化工等领域具有重要应用价值. 利用生物质资源制备含氮化合物不仅可以减少对化石资源的依赖, 而且使生物质炼制产物更加多元化. 本论文综述了近年来以生物质为原料合成含氮化合物的研究进展; 根据底物及产物结构特点, 系统介绍了从生物质平台分子包括生物质糖、糠醛、乙酰丙酸和木质素模型化合物及真实木质素为原料构建多种高附加值含氮化合物的最新研究成果; 并且对生物基含氮化合物的催化体系和反应路径进行讨论, 对该研究方向面临的主要挑战及未来趋势进行分析与展望.