Green and efficient graphitization of biomass waste empowered by molten salt electrolysis: mechanistic exploration and energy storage applications dual-driven by experiments and simulations†

IF 10.7 2区 材料科学 Q1 CHEMISTRY, PHYSICAL
Hailan Zhao, Hao Wu, Tao Rong, Jun Zhao, Mingyong Wang, Shuqiang Jiao and Haibin Zuo
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Abstract

The efficient conversion of biomass waste into graphite materials with high crystallinity and graphitization degree is one of the key ways to recycle biomass waste and obtain high value-added carbon materials sustainably. We propose a low-temperature electrochemical conversion strategy-a molten salt electrolysis graphitization process – that is simple, efficient, catalyst-free, clean, environmentally friendly, and sustainable. The method involves a direct one-step, template-free conversion of biomass waste into graphitic materials with tunable microstructures in the form of petal-like nanosheets by cathodic polarization of biomass waste in molten CaCl2 at 950 °C. The graphitization transformation mechanism was analyzed and further investigation of the potential removal mechanism of heteroatoms (e.g., oxygen, nitrogen, and sulfur) during the conversion process was carried out by experimentation and simulation. The graphitic material's unique microstructure improved lithium-ion diffusion kinetics. When applied as a negative electrode of lithium-ion batteries it delivered a specific capacity of 335.69 mA h g−1 (1C), and the reversible capacity was maintained at 340.02 mA h g−1 after 500 cycles (0.2C), with a coulombic efficiency of 99.96%. The process proposed in this paper is a coupled process integrating deoxygenation-impurity removal, defect elimination, graphitization, micro- and nano-structure construction, and self-purification, which is conducive to the establishment of a stable, closed-loop carbon cycle in the production, application, recycling and reuse of biomass waste.

Abstract Image

通过熔盐电解实现生物质废物的绿色高效石墨化:实验与模拟双重驱动的机理探索与储能应用
将生物质废弃物高效转化为高结晶度、高石墨化度的石墨材料,是实现生物质废弃物循环利用和可持续获取高附加值碳材料的关键途径之一。但传统工艺存在操作温度高、石墨化不充分、催化剂杂质易引入、后处理复杂等问题。在此,我们提出了一种简单、高效、无催化剂、清洁、环保、可持续的低温电化学转化策略——熔盐电解石墨化工艺。该方法通过在950°C的熔融CaCl2中对生物质废弃物进行阴极极化,将生物质废弃物直接一步、无模板地转化为具有花瓣状纳米片可调微观结构的石墨材料。从实验和模拟的角度分析了石墨化转化机理,并进一步研究了转化过程中杂原子(如氧、氮、硫)的潜在去除机制。其独特的微观结构促进了锂离子的扩散动力学。作为锂离子电池负极时,比容量为335.69mAh g-1 (1C),循环500次(0.2C)后,可逆容量保持在340.02mAh g-1,库仑效率为99.96%。本文提出的工艺是集脱氧-除杂、缺陷消除、石墨化、微纳米结构构建和自净化于一体的耦合工艺,有利于在生物质废弃物的生产-应用-回收再利用中建立稳定的闭环碳循环。该方法为生物质废弃物的增值利用提供了一条可持续的途径。
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来源期刊
Journal of Materials Chemistry A
Journal of Materials Chemistry A CHEMISTRY, PHYSICAL-ENERGY & FUELS
CiteScore
19.50
自引率
5.00%
发文量
1892
审稿时长
1.5 months
期刊介绍: The Journal of Materials Chemistry A, B & C covers a wide range of high-quality studies in the field of materials chemistry, with each section focusing on specific applications of the materials studied. Journal of Materials Chemistry A emphasizes applications in energy and sustainability, including topics such as artificial photosynthesis, batteries, and fuel cells. Journal of Materials Chemistry B focuses on applications in biology and medicine, while Journal of Materials Chemistry C covers applications in optical, magnetic, and electronic devices. Example topic areas within the scope of Journal of Materials Chemistry A include catalysis, green/sustainable materials, sensors, and water treatment, among others.
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