生物质多元醇水相重整制氢研究进展

生物质多元醇水相重整是一项正在发展的、很有前景的制氢技术。本文对近些年来涌现的生物质多元醇水相重整制氢研究进行了综述,讨论了多元醇水相重整反应热力学,介绍了反应动力学特征,并以此为基础对反应机理、催化剂体系以及工艺条件优化进行了总结。通过与蒸汽重整对比,指出了水相重整制氢技术的优缺点:优点是能耗低、工艺步骤较少、后处理简单;缺点是副反应多,收率低。最后,提出开发更为高效稳定的催化材料、降低催化剂制备成本和优化工艺条件将是未来研究工作的重点。     

生物质衍生磁性碳基复合材料的制备及其吸波性能

为响应国家碳中和、碳达峰目标,解决磁性碳基复合材料制备方法繁杂、能耗高、环境不友好等问题,提出生物质衍生法制备碳基吸波材料的新策略.通过选取香菇为原料,铁盐为金属源,经吸附得到铁/香菇前驱体,后经高温煅烧得到Fe/Fe4 N/C复合材料,对材料的相结构、微观形貌、热稳定性、磁特性等理化性质进行表征,分析其吸波性能.研究...     

High-Density Atomic Fe–N4/C in Tubular,Biomass-Derived,Nitrogen-Rich Porous Carbon as Air-Electrodes for Flexible Zn–Air Batteries

Developing low-cost single-atom catalysts (SACs) with high-density active sites for oxygen reduction/evolution reactions (ORR/OER) are desirable to promote the performance and application of metal–air batteries. Herein, the Fe nanoparticles are precisely regulated to Fe single atoms supported on the waste biomass corn silk (CS) based porous carbon for ORR and OER. The distinct hierarchical porous structure and hollow tube morphology are critical for boosting ORR/OER performance through exposing more accessible active sites, providing facile electron conductivity, and facilitating the mass transfer of reactant. Moreover, the enhanced intrinsic activity is mainly ascribed to the high Fe single-atom (4.3 wt.%) loading content in the as-synthesized catalyst.Moreover, the ultra-high N doping (10 wt.%) can compensate the insufficient OER performance of conventional Fe N C catalysts. When as-prepared catalysts are assembled as air-electrodes in flexible Zn–air batteries, they perform a high peak power density of 101 mW cm⁻², a stable discharge–charge voltage gap of 0.73 V for >44 h, which shows a great potential for Zinc–air battery. This work provides an avenue to transform the renewable low-cost biomass materials into bifunctional electrocatalysts with high-density single-atom active sites and hierarchical porous structure.     

Revealing Intrinsic Relations Between Cu Scales and Radical/Nonradical Oxidations to Regulate Nucleophilic/Electrophilic Catalysis

Copper/carbon catalysts under different electron-transfer regimes can evolve both radical and nonradical pathways in peroxide activation. However, the underlying trigger to manipulate the transition in between is unclear. Herein, it is revealed that Cu species in a state of sub-nanometre particles (SNPs, < 1 nm) exhibits an electrophilic nature, which is opposite to its nucleophilic nature at a larger scale (nanoclusters, > 1 nm). This switch between nucleophile/electrophile nature leads to distinct catalytic mechanisms in activating peroxymonosulfate, i.e., nonradical ¹O₂ surface-bound upon Cu SNPs and unleashed radical ^•OH induced by Cu nanoclusters. The vacancy defects of biomass-derived carbon can stabilize Cu SNPs via a Cu V C configuration, circumventing the contemporary difficulties in coordinating/preserving Metal N C bonding. Depth profiling, chemical probes, and charge density difference modeling support the regulable electroactive nature over modulated Cu scales. This featured system is applied for tetracycline degradation, and Cu SNPs demonstrates the highest efficacy with their better peroxymonosulfate confinement in nonradical regime (88.9% removal, nucleophilic activation). Comparatively, severe Cu leaching caused by radical erosion (44.8% removal, electron-donation) is undesirable. Overall, a regulable heterogeneous catalysis is unraveled over carbon-supported Cu sites through scaling modulation and defect engineering. This study illuminates a promising path for customizing biomass-derived Cu-based catalysts to achieve versatile catalysis.