Sustainable Chemistry for Climate Action
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2023
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IF 0
Ya-Qi Ba,Yong-Sheng Wang,Tian-Yi Li,Zhe Zheng,Guang-Ping Hao,An-Hui Lu
CO 2 capture from flue gas is one of the global urgent tasks. Adsorption separation of CO 2 is an energy-efficient way as compared to the absorption method. The central issue is to devise efficient adsorbents that work well under flue gas conditions with temperatures of 323–348 K and low CO 2 concentrations of 15%. In this work, we targeted this issue and proposed a well-controlled diffusion strategy, which is achieved over a series of poly(furfuryl alcohol)-derived carbons (PFCs) with dense and abundant ultra-micropores. As the adsorption temperature increased from 298 to 348 K, the CO 2 capture capacity is 54% kept for PFC-800, which is 1.2 times higher than that for samples without diffusion limitation. The capture of CO 2 is kinetics control at ambient temperature, however, at 348 K CO 2 with higher kinetic energy can overcome the restriction of the narrow pore entrance and the CO 2 /N 2 selectivity for simulated flue gas composition increases from 20 to 40. Furthermore, the PFCs exhibit a high CO 2 volumetric adsorption capacity of 97 cm 3 cm −3 at 298 K and 1 bar, benefiting the practical application deployed with an integrated adsorption column. The diffusion kinetics can be further tuned when altering the bulk phase into nanocoating, which would inspire their application in different scenarios.
研究领域:
材料科学
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环境科学
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化学工程
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DOI
ACS Sustainable Chemistry & Engineering
·
2025
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IF 7.3
Ziyang Xu,Ying Shen,Liang Chen,Chunbo Wang
Direct CO2 hydrogenation from primary carbon sources such as flue gas offers an attractive route for carbon-neutral fuel synthesis, yet the presence of O2 severely impairs catalyst performance due to preferential H2–O2 reactions and subsequent catalyst deactivation. Herein, we report a surface-engineered Ni/γ-Al2O3 (Ni/A) catalyst modified by Cu doping (Ni–Cu1/A), which exhibits enhanced oxygen resistance and sustained CH4 produce under oxidative conditions. Guided by a descriptor τ, defined as the ratio of O2 to CO2 adsorption energies, Cu was identified as an effective dopant to suppress O2 adsorption while preserving CO2 activation. Under a challenging atmosphere containing 6% O2, the optimized Ni–Cu1/A catalyst achieved a CH4 STY of 76.4 mmol gcat–1 h–1, significantly outperforming the undoped Ni/A catalyst, which drops to 63.1 mmol gcat–1 h–1 under the same conditions. Mechanistic analysis reveals that Cu incorporation weakens O2 adsorption by regulation of electronic structure, thereby mitigating exothermic H2–O2 side reactions and stabilizing Ni0 sites. This work presents a practical and scalable strategy for CO2 methanation in the presence of O2, offering a promising approach for direct catalytic conversion of flue gas by leveraging selective surface adsorption and electronic structure modulation.
研究领域:
催化
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环境化学
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材料科学
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化学工程
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产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
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2024
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IF 6.3
Huiyuan Cheng,Jingwei Hu,Zihan Liu,Guangping Lei,Guojun Xi,Yayun Zhang,Hantao Liu,Xuhuan Guo,Huiyun Ren
Developing novel adsorbents for CO 2 capture and separation offers an efficient approach to relieving global environmental problems. To promote CO 2 capture from flue gas, novel Cr 3 O@MIL-101(Cr) composites was synthesized through packing [Cr 3 O(HCOO) 6 (H 2 O) 3 ]NO 3 into MIL-101(Cr) cages. The resultant composite Cr 3 O@MIL-101(Cr) presents higher CO 2 uptakes at lower pressure ranges, benefiting from the increased content of unsaturated Cr(III) ions and micropores relative to MIL-101(Cr). Meanwhile, IAST selectivity for CO 2 /N 2 mixture reached 50.2 under standard temperature and pressure, outperforming most of the reported materials. Further GCMC simulations reveal that the synergistic effect of [Cr 3 O(HCOO) 6 (H 2 O) 3 ] + , NO 3 − and MIL-101 (Cr) could effectively facilitate the interactions with CO 2 molecules and hinder N 2 molecules from approaching the optimal adsorption sites. Thus the [Cr 3 O(HCOO) 6 (H 2 O) 3 ]NO 3 encapsulated MIL-101(Cr) can be recommended as a promising adsorbent for superior CO 2 /N 2 separation.
研究领域:
材料科学
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环境科学
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化学工程
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Peijing Shao,Zheng He,Yutao Hu,Yao Shen,Shihan Zhang,Yanan Yu
Carbonic anhydrase (CA) enzyme-based absorption processes represent a promising approach to flue gas CO 2 capture owing to their rapid absorption rates and low energy penalties. However, CA enzymes exhibit poor stability and activity under typical flue gas conditions, thus constraining their industrial utilization. Enzyme immobilization has been proposed as a potential means of improving associated stability and activity levels, thus overcoming these limitations. Herein, a variety of zeolitic imidazolate frameworks including ZIF-8, ZIF-11, and ZIF-90 with a range of organic ligands were synthesized as adsorption-based carriers for CA enzyme immobilization. In a series of experiments, CA immobilized on ZIF-8 (CA/ZIF-8) was found to retain higher activity levels that were approximately 86% of those of the free enzyme, as compared to 44% and 16% for CA/ZIF-11 and CA/ZIF-90, respectively. Immobilized CA and associated carrier frameworks were characterized via XRD, SEM, and BET. Variations in CA enzyme secondary structural characteristics in the context of immobilization were monitored via FTIR and CD to explore the molecular basis for variable activity levels associated with different carriers, revealing more hydrophilic materials to be conducive to the preservation of enzymatic activity. In addition, carrier precursor selection should take both hydrophilicity and the potential inhibitory effects of functional groups on the CA enzyme into account.
研究领域:
化学工程
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环境科学
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材料科学
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生物化学
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产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
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2025
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IF 7.2
Shuting Zhang,Jianwen Wei,Xuequan Zou,Linlin Geng,Xiaobin Zhou
This work demonstrates a strategic fabrication of high-performance CO 2 adsorbents by impregnating three conventional ionic liquids (ILs: [BMIM][NTf 2 ], [EMIM][NTf 2 ] or [EMIM][SCN]) with a covalent organic framework (COF) for carbon dioxide (CO 2 ) capture under simulated flue gas streams (1 bar, 15 vol% CO 2 , 60 ℃). Through the systematical assessment of the effects of IL structural features (different anions and cations), adding ratios (15–95 wt%), and operational temperatures (30–90 °C), it was shown that the adsorbent modified by [EMIM][SCN] in an appropriate amount (35 wt%) achieves the remarkable CO 2 adsorption capacity (5.273 mmol·g −1 at 60 ℃), representing a 3.7-fold enhancement compared to the original COF (1.419 mmol·g −1 ) due to its optimal combination of small molecular weight, short alkyl chain cation, and high CO 2 affinity anion. FTIR analysis revealed the potential adsorption mechanisms: the amine of COF chemisorbs CO 2 through carbamate formation, while the ILs enhance both chemisorption and physisorption of CO 2 via the thiocyanate nucleophilicity, the [NTf 2 ] - electronic redistribution, and hydrogen bonding of imidazolium, which is dominated by anion. The optimum CO 2 adsorption temperature (45–60 ℃) matches post-desulfurization flue gas conditions in coal-fired plants. With excellent performance and robust stability, these innovative adsorbents show practical potential for CO 2 capture in real post-combustion flue gas scenarios.
研究领域:
环境科学
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材料科学
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化学工程
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纳米技术
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产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Shudan Chi,Yi Ye,Xinglei Zhao,Junteng Liu,Junsu Jin,Le Du,Jianguo Mi
Greenhouse gases lead to frequent natural disasters, and CO 2 emissions from flue gases account for nearly half of anthropogenic CO 2 emissions. As an adsorbent, molecular sieves show excellent CO 2 adsorption; however, their defects limit their industrial application. To solve the problem of powder blockage and H 2 O absorption, we proposed the in-situ growth of molecular sieve in polyacrylate matrix beads to obtain molecular sieve composite for CO 2 capture in flue gas after combustion. Compared with those of pristine NaY, the CO 2 adsorption capacity of NaY@PA composite increased by 17.9 % and the H 2 O adsorption capacity decreased by 36.6 %. For further reduction in H 2 O absorption, post-modified composite NaY-ZIF@PA was synthesized by loading ZIF on NaY@PA surface to form a bilayer composite structure. The H 2 O absorption of NaY-ZIF@PA was reduced by 54.8 %, thus ensuring highly efficient CO 2 adsorption.
研究领域:
环境科学
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材料科学
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化学工程
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产品关联
DOI
高影响因子
CATALYSIS LETTERS
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2025
·Vol. 155
·期 10
·1-11
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IF 2.4
Zhou Jie,Yu Wen-Wang,Meng Xiang-Guang,Li Wen,Chu Dan-Dan
The development of catalytic systems capable of in situ capturing carbon dioxide (CO 2 ) from flue gas under ambient pressure and subsequently converting it into high-value chemicals holds significant practical importance for reducing atmospheric CO 2 levels and advancing the chemical industry. In this study, deep eutectic solvents (DESs) composed of an imidazolium salt and 3-aminobenzyl alcohol were synthesized and employed to catalyze the cycloaddition of CO 2 from simulated flue gas (15% CO 2 + 85% N 2 ) with epoxides. This catalytic system exhibited excellent catalytic activity, the yield of cyclic carbonate reached up to 94.3% upon reacting under simulated flue gas conditions at 55 °C and 1 atm for 24 h. The effects of temperature, reaction time and catalyst dosage on catalytic efficiency were investigated. The scope of various epoxides was also explored. Furthermore, the catalytic system is readily recyclable, maintaining nearly consistent catalytic activity over five cycles. The catalytic mechanism was clarified via FT-IR and NMR spectroscopic analyses, and a plausible cycloaddition reaction pathway was proposed. Graphical
研究领域:
绿色化学
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碳捕集与利用
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催化
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可持续能源
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材料化学
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产品关联
DOI
高影响因子
Industrial Chemistry & Materials
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2025
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IF 11.9
Bocheng Yu,Muqing Yang,Yijian Qiao,Yaozu Wang,Yongqing Xu,Xuan Bie,Qinghai Li,Yanguo Zhang,Shuzhuang Sun,Hui Zhou
Integrated carbon capture and utilization (ICCU) has emerged as a promising strategy toward carbon neutrality. However, most existing studies rely on simulated flue gas compositions, neglecting the impact of common impurities such as sulfur oxides (SOx) and nitrogen oxides (NOx), thereby limiting the practical industrial applicability of ICCU technologies. Herein, we systematically investigate the effects of SO2 and NO2 at various concentrations on the adsorption-catalysis performance based on a representative Ni-Ca dual functional material (DFM) in ICCU-dry reforming of methane (ICCU-DRM) process. Exposure to 100 ppm SO2 showed negligible influence on catalytic activity but markedly inhibited carbon deposition. Further increasing the SO2 concentration to 500 ppm led to complete deactivation of the DFM. NO2 exhibited a similar concentration-dependent trend to SO2, albeit with a comparatively lower impact. Mechanistic analysis revealed that both SO2 and NO2 promote the formation of a coating layer of calcium-containing compounds on the surface of Ni nanoparticles, accounting for the part or total deactivation. These findings offer critical insights into the industrial applications of ICCU systems under realistic flue gas conditions.
研究领域:
化学工程
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环境科学
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能源技术
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催化
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材料科学
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产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
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IF 9.965
Zhongzheng Zhang,Jialin Shi,Tianyang Zhu,Lina Zhang,Wei Wei
Fabrication of efficient heterogeneous catalysts with high turnover frequency (TOF) is intriguing for rapid and scalable CO 2 conversion under mild conditions, but it still faces some challenges due to use of some bulky and irregular supports causing inaccessible inner pores and insufficient utilization of active sites. Herein, using a unique nitrogen-doped mesoporous single-crystal carbon (named IRFC) as a host for loading Ag nanoparticles for the first time, a series of Ag/IRFC catalysts with high TOF (8.7–22.3 h −1 ) were facilely prepared by a novel “impregnation and in-situ reduction” strategy. The neat morphology and high porosity of IRFC with abundant N species, providing homogeneous surface, adequate space and anchoring sites for Ag immobilization, greatly facilitated the formation of highly-distributed ultrasmall Ag nanoparticles (2.3 nm). Meanwhile, smooth and short diffusion pathways were inherited from the ordered mesopores and small particle sizes of IRFC. Owing to these unparalleled structural features, the Ag/IRFC catalysts exhibited excellent catalytic activity, stability, and generality for mild CO 2 conversion even under diluted conditions. This work not only presents a novel catalyst for mild CO 2 conversion, but also brings some inspirations to designing highly efficient catalysts using well-shaped supporting nanomaterials for direct utilization of low-concentration CO 2 , such as flue gas.
研究领域:
催化
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材料科学
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环境化学
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DOI
高影响因子
Journal of CO2 Utilization
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2022
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IF 8.321
Jiqing Dong,Ran Ping,Xun Dai,Dongchao Wang,Fusheng Liu,Shanshan Du,Mengshuai Liu
The combination of pyrrolidine-2,5-dione-derived ionic liquids with silver acetate (AgOAc) were developed as binary catalysts for conversion of simulated flue gas CO 2 and propargylic alcohols to α-alkylidene cyclic carbonates . By tuning different catalyst components, the [HTMG][Pyrro]/AgOAc system was confirmed to be the most efficient and exhibited an excellent synergistic action in facilitating the carboxylic cyclization under room temperature and solvent-free conditions. The influence of reaction parameters on carboxylic cyclization of CO 2 with 2-methylbut-3-yn-2-ol were optimized. Under the determined conditions, the [HTMG][Pyrro]/AgOAc system was stable enough to show durable high activity in eight recycles, and also versatile in carboxylic cyclization of flue gas CO 2 with other propargylic alcohols. Moreover, a thorough comparison of [HTMG][Pyrro]/AgOAc with the reported catalysts was provided and evaluated, the results suggested that the developed catalytic system has significant advantages in practical application. Finally, the mechanistic details for the conversion of CO 2 into α-alkylidene cyclic carbonates catalyzed by [HTMG][Pyrro]/AgOAc was also elucidated on the basis of reactants activation.
研究领域:
化学
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催化
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环境科学
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材料科学
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产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
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IF 9
Fang Wang,Jinchi Mu,Zhonghai Zhang,Jixin Dong,Jinyao Han,Ruiyang Zhang,Ying Zhou
CO 2 capture is one of the most straightforward ways for solving the greenhouse gas effects. Hydrate-based CO 2 capture from flue gas has been considered as an emerging green technology owing to its low energy consumption, cost-effectiveness, and environmental benefits. In this study, the hydrophilic functionalized multi-walled carbon nanotubes (FMWCNTs) were modified and applied for CO 2 capture from flue gas by combining the dynamic experiments towards CO 2 hydrate formation and theoretical simulations. Firstly, the selective adsorption towards CO 2 in the simulated flue gas was greatly improved by regulating the hydrophilic functional groups, especially for COOH groups on the surface. Particularly, FMWCNTs induced a rapid accumulation of CO 2 , which largely shortened the hydrate nucleation time to 13 min, reducing by 59.4 % compared to the pristine THF system. This further promoted the formation of CO 2 hydrate crystals and enhanced the hydration rate and gas consumption. As a result, the CO 2 storage capacity achieved 6.48 mmol/(mol·H 2 O), with the highest separation efficiency of 76.3 %, which increased by 23.6 % and 22.7 % than that of SDS-based traditional accelerators. Particularly, the low concentration of 0.01 wt% FMWCNTs still achieved a high separation efficiency of 73.4 %, showing a great potential as kinetic accelerators with low dosage. The present study could provide novel insights into the development of modified carbon nanotubes as the kinetic accelerators for CO 2 capture.
研究领域:
环境工程
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纳米技术
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能源技术
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化学工程
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气候科学
✓ 已验证
产品关联
DOI
高影响因子
Surfaces and Interfaces
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2024
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IF 5.7
Jiawei Zhou,Ming Liu,Xue Chen,Shiyang Bai,Jihong Sun
The purification and separation of CO 2 , CH 4 , and N 2 from biogas, flue gas, and coalbed gas for carbon capture and storage are main technology in mitigating the greenhouse effect. The Mg-MOF-74@clinoptilolite (Mg-MOF-74@CP) composites are successfully synthesized through an interfacial growth of Mg-MOF-74 onto the surfaces of the synthesized CP for adsorption and separation of CO 2 , CH 4 , and N 2 . The structural characteristics of the resultant composites are systematically characterized by various characterizations. In particular, small-angle X-ray scattering (SAXS) patterns are used to elucidate the fractal structural evolutions of the parent CP, Mg-MOF-74, and Mg-MOF-74@CP. Meanwhile, the single-component adsorption isotherms for CO 2 , CH 4 , and N 2 are demonstrated. The breakthrough measurements on CO 2 /CH 4 and cycling tests on CO 2 are conducted. The results elucidate that the CO 2 equilibrium capacity of Mg-MOF-74@CP is higher than that of parent CP, displaying a high affinity toward CO 2 , the longer breakthrough time and enhancement of CO 2 uptake exhibit a better separation performance. The cycling tests on CO 2 reveal that the Mg-MOF-74@CP could be used repetitively, promoting its practical application in an energy-saving and economical way. Additionally, the adsorption isotherms and adsorption sites of the prepared Mg-MOF-74@CP are simulated using the Grand Canonical Monte Carlo (GCMC) method, elucidating the mechanism of the gas separation performance of Mg-MOF-74@CP.
研究领域:
材料科学
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化学工程
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环境科学
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吸附技术
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气体分离
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）