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原位热解太湖水华蓝藻生物质制备 CO2 吸附用多孔碳吸附剂:本征 N 的作用。

In-situ pyrolysis of Taihu blue algae biomass as appealing porous carbon adsorbent for CO capture: Role of the intrinsic N.

机构信息

School of Environmental and Civil Engineering, Jiangnan University, Wuxi 214122, PR China.

School of Environmental and Civil Engineering, Jiangnan University, Wuxi 214122, PR China; Jiangsu Key Laboratory of Anaerobic Biotechnology, Wuxi 214122, PR China; Jiangsu Collaborative Innovation Center of Technology and Material of Water Treatment, Suzhou 215011, PR China.

出版信息

Sci Total Environ. 2021 Jun 1;771:145424. doi: 10.1016/j.scitotenv.2021.145424. Epub 2021 Jan 27.

Abstract

An environment-friendly, cost-effective, and facile N self-doping porous carbon (NC) were prepared through in-situ pyrolysis of nitrogen abundant Taihu blue algae biomass for CO uptake. It was found that the CO sorption capacity of porous carbon prepared through carbonization at 800 °C with KOH activation (N-C-800) exhibit higher CO uptake capacity of 4.88 (1 bar and 0 °C) and 2.76 mmol/g (1 bar and 25 °C) respectively, with the CO/N selectivity of N-C-800 attaining 39.3. Besides, the adsorption capacity of N-C-800 remained stable even after 7 repeated cycles, with a slight loss of nearly 6%. Moreover, total graphitic N (N) sources from the intrinsic N in N-C-800 is not only higher than other agro-sourced porous carbon materials, but the graphitic N performed a sound correlation with the CO uptake capacity. Combining experiments with Density Functional Theory (DFT) calculations, higher adsorption energy of N-C-800 (-13.6 kJ/mol, comparing with -6.9 kJ/mol of N-free carbon framework) would render the efficient adsorption of CO molecular onto the graphitic N site. The current study not only provides a new option for the reclamation of Taihu blue algae biomass as N self-doping material, but a proof-of-concept investigation employing NC materials as an appealing candidate for CO capture.

摘要

通过原位热解富氮太湖水生蓝藻生物质制备了一种环保、经济且简便的 N 自掺杂多孔碳(NC)用于 CO 吸附。研究发现,在 800°C 下碳化并用 KOH 活化(N-C-800)制备的多孔碳具有更高的 CO 吸附容量,分别为 4.88(1 巴和 0°C)和 2.76 mmol/g(1 巴和 25°C),CO/N 选择性达到 39.3。此外,即使经过 7 次重复循环,N-C-800 的吸附容量仍保持稳定,仅略有损失(近 6%)。此外,N-C-800 中源自固有 N 的总石墨 N(N)含量不仅高于其他农业源多孔碳材料,而且石墨 N 与 CO 吸附容量呈良好相关性。通过实验和密度泛函理论(DFT)计算相结合的方法,N-C-800 的更高吸附能(-13.6 kJ/mol,相比之下,无 N 的碳骨架为-6.9 kJ/mol)使得 CO 分子能够有效地吸附到石墨 N 位上。本研究不仅为太湖水生蓝藻生物质作为 N 自掺杂材料的回收提供了新选择,还为 NC 材料作为 CO 捕获的有吸引力的候选材料提供了概念验证研究。

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