Journal of Environmental Chemical Engineering
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2025
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IF 7.2
Jing Bai,Chenxu Qiu,Yanhui Wang,Qianqian Zhu,Zheng Yan,Chun Chang,Pan Li,Dongyang Li
Separating CO 2 from flue gas through hydrate method owns many advantages, including easy operation, environmental friendliness, low-energy consumption during the process, and the potential for water recycling in the reaction. This study investigated the effects of cyclopentane (CP, 5.0 vol%), methionine (L-Met, 0.2 wt%), and alkyl polyglucosides (APG) with various carbon chain lengths as additives on the kinetics of flue gas hydrate generation in a simulated power plant environment, with a focus on gas separation efficiency. Key parameters, including impinging strength ( β ), feed pressure, initial temperature, and APG carbon chain length, were systematically investigated to optimize the hydrate formation process. The results reveal that gas consumption ( Δ n H ), average reaction rate ( R H ), and CO 2 capture rate ( S.Fr. (CO 2 )) initially increases with β , reaching a peak before decreasing, while the CO 2 separation factor ( S.F. (CO 2 )) consistently increased. Higher feed pressures and lower initial temperatures enhanced gas consumption, thereby accelerating the hydrate formation and improving separation efficiency. Additionally, the optimal APG carbon chain length significantly enhanced both the kinetics of hydrate formation and gas separation efficiency. Specifically, under conditions of 6 MPa, 275.15 K, and β = 0.13, the CP+L-Met+APG0814 system achieved a maximum Δ n H of 0.509 mol, an R H of 0.102 mol/h, and a S.F. (CO 2 ) of 82.4 %, demonstrating the potential for improved CO 2 capture in hydrate-based separation processes.
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Journal of Environmental Chemical Engineering
·
2024
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IF 7.4
Kang-Qi Chang,Yu-Hua Dong,Ke-Yi Liao,Ya-Chun Zeng,Yang-Yang Gou,Xiu-Guang Yi,Wei Hui,Xiao-Yu Xiao
Waste-derived porous carbon shows great potential for application in CO 2 capture and conversion. In this work, we report a modified method for upcycling waste foam from vehicular sound insulation materials into porous carbon fiber composites that can be used for efficient CO 2 capture and conversion under 1 bar conditions. The sponge-like porous carbon composites have high nitrogen content, porosity, and mechanical strength, and can selectively adsorb CO 2 from flue gas. The adsorbed CO 2 can be desorbed via heating or vacuum and then converted into useful products such as cyclic carbonates. Besides, sponge-like porous carbon composites show good stability and recyclability, and can be easily scaled up in industrial applications. It is important to note that high-temperature carbonization causes the loss of nitrogen in unmodified porous carbon materials, which makes physical adsorption the dominant type of CO 2 adsorption. In contrast, composite materials that have undergone in-situ polymerization primarily adsorb and activate CO 2 through chemical action. The results of BET, XPS, TEM, FT-IR, and DFT studies suggest that the modified sponge-like porous carbon composites with more active sites are beneficial for CO 2 capture and conversion. Therefore, this study provides a green and sustainable way to utilize waste foam from end-of-life vehicles and the value-increment of CO 2 .
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Materials
·
2024
·Vol. 17
·期 7
·1598
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IF 3.1
Yongqi Liu,Shasha Chu,Yuebing Xu,Xinyu Chen,Hao Zhou,Jinlin Li,Yanjie Ren,Xintai Su
Upcycling Cr-containing sulfate waste into catalysts for CO2hydrogenation reaction benefits both pollution mitigation and economic sustainability. In this study, FeCrO3/Fe2O3catalysts were successfully prepared by a simple hydrothermal method using Cr-containing sodium sulfate (Cr-SS) as a Cr source for efficient conversion and stable treatment of Cr. The removal rate of Cr in Cr-SS can reach 99.9% at the optimized hydrothermal conditions. When the synthesized catalysts were activated and used for the CO2hydrogenation reaction, a 50% increase in CO2conversion was achieved compared with the catalyst prepared by impregnation with a comparable amount of Cr. According to the extraction and risk assessment code (RAC) of the Reference Office of the European Community Bureau (BCR), the synthesized FeCrO3/Fe2O3is risk-free. This work not only realizes the detoxification of the Cr-SS but transfers Cr into stable FeCrO3for application in a catalytic field, which provides a strategy for the harmless disposal and resource utilization of Cr-containing hazardous waste.
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PubMed
高影响因子
Sustainable Energy & Fuels
·
2024
·Vol. 8
·期 13
·2860-2868
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IF 5
Lan-Hui Feng,Zhi-Hui Lv,Yi-Jie Kong,Xin-Ming Hu
Excessive CO2 emission and plastic waste pollution constitute two pressing threats to our environment. Effective tactics are urgently demanded to address these issues. Herein, we report that the thermal treatment of plastic wastes in the presence of nickel chloride, melamine, and KCl/LiCl salt mixture produces atomic nickel and nitrogen-doped carbon materials (Ni–N–C), which are proven to be effective for electrocatalytic CO2 conversion. We disclose that the treating temperature and the activation of molten KCl/LiCl play critical roles in fabricating Ni–N–C with high porosity, abundant Ni sites, and good charge transfer ability. As a result, Ni–N–C-800 prepared from polyethylene terephthalate bottles exhibits good performance in electrochemical CO2-to-CO conversion. Importantly, a large current density of 400 mA cm−2 and a high faradaic efficiency of 90% for CO production can be achieved in the flow cell, which endows Ni–N–C-800 with great prospects for industrial applications. Furthermore, we show that the thermal treatment of other plastic wastes such as polyethylene, polypropylene, and polyvinyl chloride can also yield effective Ni–N–C catalysts, demonstrating good universality of upcycling plastic wastes to efficient catalysts. This study puts forward a sustainable solution for the simultaneous valorization of both CO2 and plastic wastes.
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Frontiers of Chemical Science and Engineering
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2025
·Vol. 19
·期 12
·1-11
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IF 4.5
Pan Chunhong,Wang Biao,Mao Jinman,Li Mengjia,Wang Huimin,Chen Wenyi,Gao Feng,Hu Guoping,Fan Xiaolei,Huang Feng
Reverse water-gas shift reaction represents a strategic pathway for CO 2 utilization. Despite its potential, reverse water-gas shift reaction via conventional thermal-catalysis faces several challenges, including low equilibrium conversion rates due to thermodynamic constraints, high energy consumption, and insufficient product selectivity. Here, this study demonstrates an evident synergetic effect between plasma and Ag/ZnO, on enhancing reverse water-gas shift reaction. The plasma catalytic system achieved significantly improved performance with a remarkable CO 2 conversion rate of 76.5%, a high CO selectivity of 96.8% and a CO yield of 74.1%, along with an energy efficiency as high as 0.19 mmol·kJ −1 , surpassing the plasma alone system and ZnO catalytic systems. Results from X-ray photoelectron spectroscopy and Auger electron spectroscopy confirm the presence of electronic metal-support interactions between Ag and ZnO, which facilitates the formation of electron-deficient Ag sites and partially reduced ZnO x species. These reactive sites, along with oxygen vacancies created during reduction treatment, enhance the adsorption and activation of H 2 and CO 2 , offering a dominant plasma-assisted surface reaction pathway for the improved reverse water-gas shift reaction. These findings underscore the crucial role of electronic metal-support interactions in manipulating surface environments to facilitate efficient plasma-assisted catalytic reactions, with significant implications for the rational design of catalysts capable of converting CO 2 efficiently under mild conditions.
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Nature Communications
·
2025
·Vol. 16
·期 1
·1-13
·
IF 15.7
Ren Bohua,Zhang Xiaowen,Yang Leixin,Wen Guobin,Dong Silong,Xiong Haoyang,Liu Yiyin,Duan Xiaoman,Tan Lichao,Wang Xin,Chen Zhongwei
Electrocatalytic upgrade of CO 2 offers a promising approach for recycling of global CO 2 emissions, facilitating the achievement of carbon neutrality. Nevertheless, direct utilization of practical dilute CO 2 is urgently important yet rather difficult, which is hindered by the balance of reaction kinetics and mass transport of CO 2 to the catalytic sites. Herein, we propose coordinating the local environment and active catalyst by constructing covalent organic frameworks (COF) on single-atomic In-doped Cu 2 O (In 1 @Cu 2 O) for a high tolerance of CO 2 inlet concentrations (15% to 100%). The optimized amounts of COF functionalized by the trifluoromethyl group act as the local CO 2 /CO diffusion channels via steric confinement effects and C···F electronic effects. Besides, the formation of key intermediates for C 2+ products is greatly facilitated by the promoted COOH adsorption. Hence, a total current of 81.7 A is realized in a 4 × 100 cm 2 electrolyzer stack with over 770 mmol/h C 2+ products at an inlet of dilute CO 2 . Such a electrode architecture sheds light on the dilute CO 2 electrolysis at the potential industrial scale.
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高影响因子
ACS Nano
·
2022
·
IF 18.027
De-Hui Guan,Xiao-Xue Wang,Fei Li,Li-Jun Zheng,Ma-Lin Li,Huan-Feng Wang,Ji-Jing Xu
At present, photoassisted Li–air batteries are considered to be an effective approach to overcome the sluggish reaction kinetics of the Li–air batteries. And, the organic liquid electrolyte is generally adopted by the current conventional photoassisted Li–air batteries. However, the superior catalytic activity of photoassisted cathode would in turn fasten the degradation of the organic liquid electrolyte, leading to limited battery cycling life. Herein, we tame the above limitation of the traditional liquid electrolyte system for Li-CO2 batteries by constructing a photoassisted all-solid-state Li-CO2 battery with an integrated bilayer Au@TiO2/Li1.5Al0.5Ge1.5(PO4)3 (LAGP)/LAGP (ATLL) framework, which can essentially improve battery stability. Taking advantage of photoelectric and photothermal effects, the Au@TiO2/LAGP layer enables the acceleration of the slow kinetics of the carbon dioxide reduction reaction and evolution reaction processes. The LAGP layer could resolve the problem of liquid electrolyte decomposition under illumination. The integrated double-layer LAGP framework endows the direct transportation of heat and Li+ in the entire system. The photoassisted all-solid-state Li-CO2 battery achieves an ultralow polarization of 0.25 V with illumination, as well as a high round-trip efficiency of 92.4%. Even at an extremely low temperature of −73 °C, the battery can still deliver a small polarization of 0.6 V by converting solar energy into heat to achieve self-heating. This study is not limited to the Li–air batteries but can also be applied to other battery systems, constituting a significant step toward the practical application of all-solid-state photoassisted Li–air batteries.
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CHEMICAL ENGINEERING JOURNAL
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2025
·
IF 13.2
Xuanang Fu,Huajie Qiu,Anteng Dai,Qinghai Long,Chao Liu,Zuoming Zhou,Guohua Jing,Bihong Lv
Achieving carbon neutrality demands advanced CO 2 capture technologies that overcome the limitations of conventional amine-based solvents, such as high energy consumption and environmental toxicity. Here, a task-specific deep eutectic solvent (DES) engineered for on-demand CO 2 capture and release, combining high efficiency, low energy consumption, and environmental sustainability was reported in this work, which employing an ionic liquid as a hydrogen bond acceptor (HBA) and ethanol as a dual-function solvent/hydrogen bond donor (HBD). The [AEP][Pro]-Ethanol system achieved a high capacity of 1.10 mol CO 2 ·mol absorbent −1 while a low viscosity of 13.06 mPa·s after saturated absorption, and kept 87 % regeneration efficiency after five regeneration cycles at 363.15 K. Mechanistic insights from combined experimental characterization and density functional theory (DFT) calculations revealed a unique CO 2 absorption pathway, enabling ultralow regeneration energy (1.94 GJ·ton −1 CO 2 )—nearly 50 % lower than monoethanolamine (MEA, 3.77 GJ·ton −1 CO 2 ). This DES platform merges molecular tunability, exceptional cycling stability, and industrial scalability, offering a breakthrough solution for next-generation carbon capture technologies.
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CHEMICAL ENGINEERING JOURNAL
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2025
·
IF 13.2
Li-Ning Dong,Cunmin Wang,Le Bao,Kun Yu,Yuzhen Hou,Xinjian He,Mengbao Fan,Shenghui Zhang,Shu-Gui Yang,Jiefeng Gao,Huan Xu
Biodegradable poly(lactic acid) (PLA) nanofibrous membranes (NFMs) alleviate plastic pollution and attract attention in particulate matter (PM) filtration. However, they lack gas selectivity, and their poor electroactivity coupled with rapid charge dissipation leads to unstable PM filtration efficiency, which hampers their further development. Herein, we employed a microwave-assisted method to fabricate high-selectivity active nanocrystals (HSANs), and integrated them into PLA NFMs via a combined electrospinning-electrospray strategy, yielding HSA-PLA NFMs with a hierarchical porous structure. With uniform HSANs anchoring (3, 6 and 9 wt%), the obtained HSA-PLA NFMs showed increased surface potential (up to 8.3 kV), dielectric constant (1.71) and porosity (95.6 %). They exhibited excellent CO 2 adsorption and HSA-PLA9 reached 1.9 mmol·g −1 at 273.15 K/1.0 bar. Its CO 2 /N 2 selectivity was confirmed by IAST/breakthrough tests and the mechanism analyzed via three isothermal models. Moreover, endowed with pronounced activity and optimized morphology, HSA-PLA NFMs exhibited PM 2.5 and PM 0.3 filtration efficiencies of 99.7 % and 99.3 % at 85 L/min, remarkably outperforming Pure PLA (only 84.9 % and 83.9 %). This strategy integrates CO 2 adsorption and PM filtration, thereby facilitating the development of eco-friendly multifunctional permselective membranes for simultaneous purification.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2025
·
IF 3.9
Peiyao Niu,Tianyou Li,Qizheng Zhao,Yongchao Sun,Jingfa Zhang,Fangxu Fan,Gaohong He,Canghai Ma
Mixed matrix membranes (MMMs) integrate the benefits of organic polymer membranes with porous inorganic fillers, leading to an enhancement in both gas permeability and separation selectivity. As a commonly used filler, ZIF-8 exhibits promise in enhancing the gas separation performance of MMMs. However, further improving the gas selectivity of ZIF-8-based MMMs remains a challenge. To improve the gas selectivity of ZIFs, we synthesized ZIF-BI via the “mixed linker method” using a bulky benzimidazole ligand, which restricts imidazole ring twisting and enhances gas selectivity. At a 40 wt % ZIF-BI loading, the ZIF-BI/6FBDA MMM exhibited CO2 and H2 permeabilities of 25.7 and 49.6 Barrer, respectively. Additionally, the CO2/CH4 and H2/N2 selectivities reached 151.4 and 261.1, both transcending the 2008 Robeson upper bounds. This work provides an innovative way to make ZIF materials and high-performance gas separation membranes, offering solutions for CO2 capture and H2 separation.
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Journal of Materials Chemistry A
·
2025
·
IF 9.5
Lili Wan,Linxiao Wu,Yumeng Han,Fusong Kang,Dongfeng Du,Jinshui Cheng,Jingshan Luo
Efficient and selective photoelectrochemical CO2 reduction remains a significant challenge for solar fuel production. Here, we fabricated a heterostructured Cu2O photocathode featuring a pristine SnO2 layer deposited via atomic layer deposition. Upon photoelectrochemical activation, the SnO2 layer transformed into uniformly distributed Sn/SnOₓ nanoparticles across the photocathode surface. Systematic characterization revealed the SnO2 layer's structural evolution. The activated Cu2O photocathode significantly enhanced the charge transfer characteristics and PEC CO2 reduction performance, delivering a current density of -2.5 mA cm-2 at -0.2 V vs. RHE and a formate Faradaic efficiency of 75.4% at -0.1 V vs. RHE. Coupling with a semitransparent BiVO4/NiCo LDH photoanode enables unassisted, solar-driven CO2 reduction and ethylene glycol (EG) oxidation, achieving a current density of 0.11 mA cm-2 and producing 0.13 μmol cm-2 formate yield in the first 0.5 hour. This work presents a scalable and earth-abundant materials-based strategy for efficient PEC CO2 reduction and underscores the potential of tandem architectures for sustainable solar fuel generation.
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CHEMICAL PHYSICS
·
2025
·
IF 2.4
Qiqi Niu,Yiqi Pan,Ming Chen,Longfei Sun,Kang Zhang,Yun Zhang,Jing Yan,Wei Qi,Lin Yang,Zhaoxia Dong,Xiaochen Li
CO 2 foam plays a pivotal role in the synergistic integration of enhanced oil recovery and carbon geological storage, which is attributed to its ability to control CO 2 mobility and accelerate CO 2 dissolution-mineralization. However, foams are inherently thermodynamically unstable systems. Notably, CO 2 not only undergoes inter-bubble diffusion but also dissolves in aqueous phases, collectively exacerbating foam destabilization. Therefore, it is of great significance to optimize the structure of the foam agent for constructing a highly stable CO 2 foam system. In this paper, the properties of CO 2 bubble film and the arrangement of molecules on the liquid film were studied through experiments and molecular simulations in a series of conventional surfactant solutions. Specifically, the effects of hydrophobic carbon chains and hydrophilic groups of surfactants on liquid film permeability, interfacial adsorption process, bubble stability, and CO 2 molecular behavior were analyzed. The lab results show that the CO 2 bubbles in systems containing C16-based quaternary ammonium (TAC-16) and betaine (S16) surfactants exhibited lifespans of 186 and 69 min, respectively, representing 85 and 29 times longer than that of C12-based counterparts (TAC-12 and S12). The liquid film permeability of CO 2 bubbles in TAC-16 and S16 were 5.02 and 11.99 cm/min, corresponding to 1/7 and 1/3 of TAC-12 and S12. Furthermore, the adsorption capacities of TAC-16 and S16 were 1.63 and 3.06 mol/m 2 at the gas-liquid interface, which were greater than those of TAC-12 and S12. Long-chain surfactants had strong hydrophobic interactions, which enhanced their adsorption and micelle formation capabilities. Long-chain surfactants showed a certain affinity for CO 2 molecules and could form a dense adsorption layer at the gas-liquid interface. The results indicate that the long-chain surfactants can delay the diffusion and dissolution of CO 2 in the liquid film and have obvious advantages as CO 2 foam agents. This work preliminarily reveals the molecular states and interactions within CO₂ foams, providing critical insights for designing and developing CO 2 foam agents.
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