有机固废高值化为CO2吸附剂研究进展：交叉研究综述

doi:10.16085/j.issn.1000-6613.2023-1544

化工进展 ›› 2024, Vol. 43 ›› Issue (10): 5748-5764.DOI: 10.16085/j.issn.1000-6613.2023-1544

• 资源与环境化工 • 上一篇

有机固废高值化为CO₂吸附剂研究进展：交叉研究综述

黄致新¹(), 王珺瑶², 袁湘洲³, 邓帅¹(), 赵洁⁴, 张欣懿¹

^1.中低温热能高效利用教育部重点实验室，天津 300350
^2.广东工业大学材料与能源学院，广东广州 510006
^3.东南大学能源与环境学院，能源热转换及其过程测控教育部重点实验室，江苏南京 210096
^4.新加坡国立大学工程学院化学与生物分子工程系，新加坡肯特岗 119260

收稿日期:2023-09-04 修回日期:2023-11-16 出版日期:2024-10-15 发布日期:2024-10-29
通讯作者: 邓帅
作者简介:黄致新（2001—），男，硕士研究生，研究方向为生命周期评价。E-mail：zhixinhuang@tju.edu.cn。
基金资助:
国家自然科学基金青年项目(72104257);天津市自然科学基金重点项目(22JCZDJC00540)

Research advances on upcycling organic solid waste into CO₂ adsorbents: A cross-research review

HUANG Zhixin¹(), WANG Junyao², YUAN Xiangzhou³, DENG Shuai¹(), ZHAO Jie⁴, ZHANG Xinyi¹

^1.Key Laboratory of Efficient Utilization of Low and Medium Grade Energy，Tianjin 300350，China
^2.School of Materials and Energy, Guangdong University of Technology，Guangzhou 510006，Guangdong, China
^3.Ministry of Education of Key Laboratory of Energy Thermal Conversion and Control, School of Energy and Environment, Southeast University, Nanjing 210096, Jiangsu, China
^4.Department of Chemical and Biomolecular Engineering，Faculty of Engineering，National University of Singapore，Kent Ridge Crescent 119260，Singapore

Received:2023-09-04 Revised:2023-11-16 Online:2024-10-15 Published:2024-10-29
Contact: DENG Shuai

摘要/Abstract

摘要：

碳捕集技术对于实现碳中和目标不可或缺。特别地，将有机固体废弃物高值化为多孔炭吸附剂并捕集CO₂，被认为是一种能够同时缓解气候变化以及固废污染的可持续方法，因此其吸附剂的合成与应用得到广泛关注。近年来，除化工、材料、热工研究方法外，在该领域内许多学者应用分子模拟、机器学习、生命周期评价等研究方法，在固废高值化为CO₂吸附剂方面进行了卓有特色的交叉研究。然而，上述交叉研究仍较为分散，缺乏脉络总结，其丰厚潜力还未得到系统阐明。本文综述了固废高值化为多孔炭吸附剂的研究进展，除常规工艺方法、制取吸附剂的性能水平外，侧重于展示该领域中应用的交叉研究，包含分子模拟、机器学习、生命周期评价三方面。本文通过脉络梳理可为该领域内交叉研究的潜在发展方向提供指引。

关键词: 碳中和, 多孔炭, 碳捕集, 分子模拟, 机器学习, 生命周期评价

Abstract:

Carbon capture technologies is indispensable to achieve carbon neutrality goals. In particular, upcycling organic solid waste into porous carbon materials for capturing CO₂ is a sustainable and practical approach that simultaneously mitigates climate change and solid waste pollutions, and thus the syntheses and applications of its adsorbents have been extensively explored. In recent years, in addition to chemical engineering, material science and thermal engineering research methods, many scholars in this field have used molecular simulation, machine learning, life cycle assessment and other research methods to carry out distinctive cross-research on valorization of organic solid waste into CO₂ adsorbents. However, the above-mentioned cross-cutting research is still relatively scattered, lacking a contextual summary, and its rich potential has not been systematically elucidated. This review addressed the research advances on upcycling organic solid waste into porous carbons for adsorbing CO₂. In addition to the conventional process methods and the performance level of the adsorbents, it focused on the application of cross-research in this field, mainly including molecular simulation, machine learning and life cycle assessment. This review provided valuable guidelines for the potential development direction of cross-research in this field through contextual analyses.

Key words: carbon neutral, porous carbon, carbon capture, molecular simulation, machine learning, life cycle assessment

中图分类号:

X705

黄致新, 王珺瑶, 袁湘洲, 邓帅, 赵洁, 张欣懿. 有机固废高值化为CO₂吸附剂研究进展：交叉研究综述[J]. 化工进展, 2024, 43(10): 5748-5764.

HUANG Zhixin, WANG Junyao, YUAN Xiangzhou, DENG Shuai, ZHAO Jie, ZHANG Xinyi. Research advances on upcycling organic solid waste into CO₂ adsorbents: A cross-research review[J]. Chemical Industry and Engineering Progress, 2024, 43(10): 5748-5764.

图/表 11

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原料	炭化方法	炭化温度 /℃	活化剂	活化温度 /℃	表面改性剂	吸附容量（25℃，1bar） /mmol·g^-1	动态吸附容量 /mmol·g^-1	选择性（CO₂-N₂）/%
菠萝废弃物^[27]	水热炭化	210	草酸锂、草酸钠、草酸钾	700	—	4.25	0.93	18.4~38.4
腐烂草莓^[28]	水热炭化	180	KOH	650	—	4.49	—	20
菊君草^[29]	水热炭化	250	KOH	700	—	4.90	—	—
山茶花^[29]	水热炭化	250	KOH	700	—	5.00	—	—
中药固废^[30]	水热炭化	270	KOH	600~800	尿素	4.02	—	21.26
虾壳^[31]	热解	400	KOH	700	—	4.20	—	23
荷叶^[32]	热解	500	NaNH₂	450~550	NaNH₂	3.5	0.82	21
榛子壳^[32]	热解	500	NaNH₂	500~600	NaNH₂	4.23	1.00	17
菱角壳^[32]	热解	500	KOH	550~650	硫脲	4.34	0.89	22
玉米芯^[33]	—	700	—	—	PEI	4.75（20℃）	2.6~2.7	—
莲杆^[34]	热解	1000	K₂CO₃/KHCO₃	80	—	—	—	—
甘蔗渣^[35]	热解	600	KOH	600	尿素	4.8	—	22
	水热炭化	240	KOH	800	乙酸	4.47	—	21.5
稻壳^[36-37]	—	520	KOH	710	—	4.16	—	—
	—	200	KOH	700	PEI	4.50	—	—
藻类^[38-39]	热解	400~800	KOH	400~800	—	0.37~1.05	—	—
	热解	800	KOH	600	尿素	3.44	—	—
	热解	800	KOH	600	尿素	3.94	—	—
椰子壳^[40-44]	热解	500	KOH	600	—	4.23	—	—
	热解	800	CO₂	800	—	3.90	—	—
	热解	500	K₂CO₃	600	尿素	4.70	—	11
	热解	500	KOH	650	尿素	4.80	—	15
	热解	500	KOH	650	氨	4.26	—	—
PET废塑料^[5,16,23,45]	热解	700	KOH	700	—	—	2.31	—
	热解	600	KOH	700	—	4.42	3.31	14
	热解	600	KOH	700	尿素	4.58	3.51	19
	热解	600	CO₂	900	—	3.63	2.68	—

原料	炭化方法	炭化温度 /℃	活化剂	活化温度 /℃	表面改性剂	吸附容量（25℃，1bar） /mmol·g^-1	动态吸附容量 /mmol·g^-1	选择性（CO₂-N₂）/%
菠萝废弃物^[27]	水热炭化	210	草酸锂、草酸钠、草酸钾	700	—	4.25	0.93	18.4~38.4
腐烂草莓^[28]	水热炭化	180	KOH	650	—	4.49	—	20
菊君草^[29]	水热炭化	250	KOH	700	—	4.90	—	—
山茶花^[29]	水热炭化	250	KOH	700	—	5.00	—	—
中药固废^[30]	水热炭化	270	KOH	600~800	尿素	4.02	—	21.26
虾壳^[31]	热解	400	KOH	700	—	4.20	—	23
荷叶^[32]	热解	500	NaNH₂	450~550	NaNH₂	3.5	0.82	21
榛子壳^[32]	热解	500	NaNH₂	500~600	NaNH₂	4.23	1.00	17
菱角壳^[32]	热解	500	KOH	550~650	硫脲	4.34	0.89	22
玉米芯^[33]	—	700	—	—	PEI	4.75（20℃）	2.6~2.7	—
莲杆^[34]	热解	1000	K₂CO₃/KHCO₃	80	—	—	—	—
甘蔗渣^[35]	热解	600	KOH	600	尿素	4.8	—	22
	水热炭化	240	KOH	800	乙酸	4.47	—	21.5
稻壳^[36-37]	—	520	KOH	710	—	4.16	—	—
	—	200	KOH	700	PEI	4.50	—	—
藻类^[38-39]	热解	400~800	KOH	400~800	—	0.37~1.05	—	—
	热解	800	KOH	600	尿素	3.44	—	—
	热解	800	KOH	600	尿素	3.94	—	—
椰子壳^[40-44]	热解	500	KOH	600	—	4.23	—	—
	热解	800	CO₂	800	—	3.90	—	—
	热解	500	K₂CO₃	600	尿素	4.70	—	11
	热解	500	KOH	650	尿素	4.80	—	15
	热解	500	KOH	650	氨	4.26	—	—
PET废塑料^[5,16,23,45]	热解	700	KOH	700	—	—	2.31	—
	热解	600	KOH	700	—	4.42	3.31	14
	热解	600	KOH	700	尿素	4.58	3.51	19
	热解	600	CO₂	900	—	3.63	2.68	—

材料	孔隙形状	表面化学组成	模拟方法	相互作用势	模拟条件	参考文献
多孔炭	多孔材料	氢、羟基团、醚、酯	GCMC	Compass	298K	[5]
石墨层	狭缝型孔隙	吡啶N、羧基团	GCMC	Lennard-Jones	273~304K	[55]
多孔炭	纳米管	羧基团	GCMC	Lennard-Jones	119.8K	[56]
多孔炭	蜂窝状	C-H group	GCMC	Lennard-Jones	318.15K	[57]
多孔炭	纳米管	—	GCMC	Lennard-Jones	300K	[58]
煤炭	层状堆叠	—	MD	GROMOS	312~394K	[59]
多孔炭	多孔球	—	GCMC	Lennard-Jones	—	[60]
多孔炭	片状	硫、氮掺杂	MD	CVFF	365K	[61]
石墨烯层	狭缝型纳米孔隙	—	MD	Lennard-Jones	353~413K	[62]
多孔炭	纳米管	羧、羰、羟基团	GCMC	Lennard-Jones; Coulomb	298K	[63]
煤炭	多孔材料	硫、氮掺杂	MD	Lennard-Jones	298K，313K，373K	[64]
多孔炭	纳米管	氢、羟、胺、羧基团	GCMC	Lennard-Jones；Columbic	298K，313K，373K	[65]

材料	孔隙形状	表面化学组成	模拟方法	相互作用势	模拟条件	参考文献
多孔炭	多孔材料	氢、羟基团、醚、酯	GCMC	Compass	298K	[5]
石墨层	狭缝型孔隙	吡啶N、羧基团	GCMC	Lennard-Jones	273~304K	[55]
多孔炭	纳米管	羧基团	GCMC	Lennard-Jones	119.8K	[56]
多孔炭	蜂窝状	C-H group	GCMC	Lennard-Jones	318.15K	[57]
多孔炭	纳米管	—	GCMC	Lennard-Jones	300K	[58]
煤炭	层状堆叠	—	MD	GROMOS	312~394K	[59]
多孔炭	多孔球	—	GCMC	Lennard-Jones	—	[60]
多孔炭	片状	硫、氮掺杂	MD	CVFF	365K	[61]
石墨烯层	狭缝型纳米孔隙	—	MD	Lennard-Jones	353~413K	[62]
多孔炭	纳米管	羧、羰、羟基团	GCMC	Lennard-Jones; Coulomb	298K	[63]
煤炭	多孔材料	硫、氮掺杂	MD	Lennard-Jones	298K，313K，373K	[64]
多孔炭	纳米管	氢、羟、胺、羧基团	GCMC	Lennard-Jones；Columbic	298K，313K，373K	[65]

材料	表面化学组成	模拟方法	CO₂吸附能/kJ·mol^-1	机制	参考文献
多孔炭	N/O共掺杂	DFT	-29.34	氮氧协同增加表面吸附的范德华作用	[66]
多孔炭球	N掺杂、O掺杂	DFT	-21.5	氧掺杂表面亲和力比氮掺杂表面亲和力弱	[67]
石墨层	N、P、S、O掺杂	DFT/GCMC	-34.42	表面极性官能团的氢键相互作用增强CO₂吸附性能	[68]
C₉N₇	N掺杂	DFT/GCMC	-26.32	层间距与CO₂吸附性能相关	[69]
多孔炭	Co掺杂、吡咯掺杂	DFT	-21.4	表面与CO₂没有明显电荷转移，阐明物理吸附机制	[70]
多孔炭	N/O共掺杂	DFT/GCMC	-35.1	高氧含量表面掺杂氮增强静电相互作用	[71]
C₃N	B掺杂、P掺杂	DFT	-30.53	磷掺杂表面的异质电荷密度分布和C、P原子的p轨道杂化	[72]
石墨炔	Sc掺杂、Cr掺杂	DFT	-23.23	多金属共修饰的石墨炔具有协同作用	[73]
多孔炭	N/O共掺杂	GCMC	-39.4	孔径增大和氮氧掺杂增强CO₂吸附性能	[74]
石墨烯	N掺杂	DFT	-34.75	负电荷密度增强氮掺杂表面的相互作用	[75]

有机固废高值化为CO₂吸附剂研究进展：交叉研究综述

Research advances on upcycling organic solid waste into CO₂ adsorbents: A cross-research review

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年份	吸附剂类型	输入特征	预测指标	算法	数据集大小	预测效果
2018^[81]	AC	T、P、比表面积、孔体积	CO₂吸附量	LSSVM	104	R²>0.89
2019^[82]	PC	S_bet、V_micro、V_meso、V_total、T、P	CO₂吸附量	ANN	1000	R²>0.9
2019^[79]	PC	S_bet、V_micro、V_meso、T、P	CO₂、N₂吸附量	ANN	1138	R²=0.96
2019^[83]	AC	比表面积、V_micro、T、P	CO₂, CH₄, N₂及其混合物吸附量	ANN	40~417	R²>0.99
2020^[80]	PC	N₂等温线、T、P	CO₂ 、N₂吸附量	CNN	679	—
2020^[84]	BWDPC	C、N、O、H、T、P、S_bet、V_micro、V_meso、V_ultra	CO₂吸附量	RF	6244	0.43(省略 k)
2020^[85]	AC	P、T	CH₄、CO₂、N₂吸附量	ANN	—	R²=0.997~0.999
2020^[86]	水炭、热解炭	C、H、N、O、FC、A、V、t_H、T_H、C_W、T_P、PHR、t_P	HHV、ER、ED	SVM	248	R²=0.90,0.94
2021^[18]	BWDPC	S_bet、V_total、V_micro、C、O、H、N、T、P	CO₂吸附量	GBDT	527	R²=0.84
2021^[87]	BWDPC	碳前体、活化剂、T_P、孔体积、P、T	比表面积、CO₂吸附量	ANN	421	R²>0.99
2022^[88]	AC、碳分子筛	P、T、吸附剂类型（等温线数据）	N₂、N₂O、O₂吸附量	ANN	1242	R²=0.993~0.996
2022^[89]	AC、沸石	P、（303K）	Ar, Xe, Kr, O₂吸附量	ANN	1400	R²=0.9978~0.9998
2022^[90]	BWDPC	V_micro、V_meso、S_bet、T、P	CO₂吸附量	ANN	500	0.43(省略 k)
2023^[91]	生物炭	T_P、C、H、O、N、S_bet、V_total、V_micro	CO₂吸附量	LGBM	334	R²=0.94
2023^[92]	PC	V_total、V_micro、V_ultra、S_bet、O、N、T、P	CO₂吸附量	RF	1594	R²>0.97

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