Xiaohua Wang, Hongfan Zhao, Yebin Zhou, Chunyu Yin, Wei He, Feng Feng, Fengli Wang, Chunshan Lu and Xiaonian Li
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引用次数: 0
摘要
生物质为获得环境友好型碳材料提供了一种前景广阔的碳源,但以绿色方法直接从生物质中获得掺杂杂原子的碳材料(HDCMs)仍然具有挑战性。本研究利用可再生酵母与水混合后在 800 至 950 °C 的温度下进行简单的原位热解,成功合成了氮磷共掺杂多孔碳材料(Y-NPC)。各种表征方法表明,氮和磷掺杂在碳骨架中,主要以石墨-N、吡啶-N、C-P、P-N 和 P-O 状态存在。催化剂 Y-NPC-900 °C 具有三维分层多孔结构和高 P-N 含量,在温和条件下以分子氢和水合肼为氢源,具有优异的硝基加氢性能和反应稳定性。密度泛函理论(DFT)计算和实验表明,N、P 共掺杂碳(NPC)的氢活化和对基质的良好吸附能力是其优异催化性能的主要原因。因此,本研究提出了一种环保、简单的生物质原位 N、P 共掺杂无金属碳催化剂合成策略,显示了 N、P 共掺杂和单一 N 或 P 单掺杂在碳材料电荷分布中的重要作用。
Yeast-derived N, P co-doped porous green carbon materials as metal-free catalysts for selective hydrogenation of chloronitrobenzene†
Biomass provides a promising source of carbon for obtaining environment-friendly carbon materials, but obtaining heteroatom-doped carbon materials (HDCMs) from biomass directly by a green method still remains challenging. This study successfully synthesized nitrogen and phosphorus co-doped porous carbon materials (Y-NPC) by the simple in situ pyrolysis of renewable yeast mixed with water from 800 to 950 °C. Various characterization methods show that nitrogen and phosphorus are doped into the carbon skeleton and mainly exist in the forms of graphite-N, pyridine-N, C–P, P–N, and P–O states. The catalyst Y-NPC-900 °C with a 3D hierarchical porous structure and high P–N content exhibited superior nitro hydrogenation performance and reaction stability using molecular hydrogen and hydrazine hydrate as hydrogen sources under mild conditions. Density functional theory (DFT) calculations and experiments attributed the exceptional catalytic performance to hydrogen activation and the good adsorption ability of substrates over N, P co-doped carbon (NPC). Therefore, this research proposes an eco-friendly and simple synthesis strategy for in situ N, P co-doping metal-free carbon catalysts derived from biomass, showing the significance of N, P co-doping and single N- or P-monodoping in the charge distribution of carbon materials.
期刊介绍:
Green Chemistry is a journal that provides a unique forum for the publication of innovative research on the development of alternative green and sustainable technologies. The scope of Green Chemistry is based on the definition proposed by Anastas and Warner (Green Chemistry: Theory and Practice, P T Anastas and J C Warner, Oxford University Press, Oxford, 1998), which defines green chemistry as the utilisation of a set of principles that reduces or eliminates the use or generation of hazardous substances in the design, manufacture and application of chemical products. Green Chemistry aims to reduce the environmental impact of the chemical enterprise by developing a technology base that is inherently non-toxic to living things and the environment. The journal welcomes submissions on all aspects of research relating to this endeavor and publishes original and significant cutting-edge research that is likely to be of wide general appeal. For a work to be published, it must present a significant advance in green chemistry, including a comparison with existing methods and a demonstration of advantages over those methods.