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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

Carbon sequestration during Fe(III)-Fulvic acid coprecipitation and kinetics of hydrated Cu(II)

Yihao Li,Hongmei Tang,Xiangqin Peng,Shiyang Tao,Jie Ding,Meiqing Chen,Pingxiao Wu,Nengwu Zhu

The dynamic interactions among iron (Fe) oxides and organic matter (OM) play vital roles in controlling the geochemical cycling of carbon (C) and toxic trace metals. Although the effects of OM on the Fe oxides transformation, and dynamic with toxic trace metals have been studied previously, it is still poor to understand the mechanistic and quantitative on the C sequestration during the Fe(III) mineralization process, and kinetics with hydrated Cu(II) in the acid drainage. In this study, Mössbauer spectroscopy, X-ray absorption spectroscopy (XAS), high resolution transmission electron microscopy (HRTEM), and density functional theory (DFT) were used to elucidate the underlying mechanism for the fine structure of iron minerals, fulvic acid (FA) sequestration and hydrated Cu(II) coordination on Fe oxides. FA dosages played an essential role in the formation of Fe oxides, which can inhibit the formation of Fe-O octahedrons and benefit to the Fe-O tetrahedron. FA molecules were mainly sequestrated on the surfaces of Fe oxides and van der Waals forces were the main interaction between FA and Fe oxides. The hydrated Cu(II) oxides mainly distributed on the surface of iron oxides as divalent oxidation states, and feasible coordinated with phenolic hydroxyl group of FA and Fe oxides. The knowledge of the dynamic coupling between Fe oxide transformation under the effect of FA and the fate of hydrated Cu(II) on Fe oxides provided the basis for predicting the geochemical process of Fe, C and toxic trace metals.

研究领域: 环境科学 · 地球化学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2024 · IF 8.1

Integration of CO2 sequestration with the resource recovery of red mud and carbide slag

Gangan Wang,Chaoyi Chen,Junqi Li,Yuanpei Lan,Xin Lin

Red mud and carbide slag, strongly alkaline solid wastes, are produced during the manufacturing of alumina and acetylene gas, respectively. Improper management of these wastes can pose significant environmental hazards. This study proposed a novel method for the collaborative treatment of red mud and carbide slag, enabling the recovery of constituent elements with CO 2 sequestration. During the hydrochloric acid leaching process, Si was reclaimed as Si-rich residue, whereas Ti, Al, Ga, Fe, and Sc were stepwise recovered as Ti-rich product, Al/Ga-rich filtrate, and Fe/Sc-rich product via the subsequent hydrolysis, co-precipitation, and alkali leaching processes, respectively. Utilizing carbide slag to replace the energy-intensive NaOH for pH adjustment in the leaching solution resulted in a Ca 2+ concentration of 21,922 mg/L in the filtrate after co-precipitation. Through further mineralization process, CO 2 sequestration was achieved alongside the production of CaCO 3 with the content reaching 98.5 % along with a whiteness of 94.4 %. Furthermore, by adjusting the experimental parameters in the mineralization process, controlled manipulation of the phase and morphology of the CaCO 3 product could be achieved to meet various industry requirements. To summarize, the complete resource recovery of red mud and carbide slag was achieved in this study, demonstrating the promising potential in practical applications.

CAS / MDL: 497-19-8 7647-01-0
研究领域: 环境科学 · 材料科学
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JOURNAL OF ENVIRONMENTAL MANAGEMENT · 2023 · IF 8.7

Enhanced sequestration of CO2 from simulated electrolytic aluminum flue gas by modified red mud

Xingyuan Wang,Jiamin Qi,Hengxi Zhu,Jiancheng Wang,Heping Zeng,Bin Li,Si Yan

The aluminum industry is facing severe economic and environmental problems due to increasing carbon emissions and growing stockpiles of red mud (RM). RM is a strongly alkaline, high-emission solid waste from the alumina industry with potential for CO 2 sequestration. However, the effectiveness of RM carbon sequestration is poor, and the mechanism behind it is not well understood. In this study, the effect of microwave and tube furnace activation of RM on CO 2 sequestration in alumina was first investigated at different temperatures. The result showed that the CO 2 sequestration capacity of unmodified RM (URM) was only 14.35 mg/g at ambient temperature and pressure, and the CO 2 sequestration capacity could be increased to 52.89 mg/g after high-temperature activation and modification. Besides, high-temperature activation and modification will effectively improve the carbon sequestration capacity of RM. The carbonized RM was characterized by FT-IR, SEM, XRD , laser particle size, TG-DSC, and pH measurements. In addition, the mechanism of RM capturing CO 2 was also proposed, which shows that CO 2 was finally sequestered in the RM as CaCO 3 . The change in particle size distribution and the mineral phase in the RM indicated that high-temperature activation modification positively affects the application of RM to the sequestration of CO 2 . This study can provide a promising technology for the low-carbon and green development of the aluminum industry, as well as achieving the waste treatment and utilization objective.

CAS / MDL: 1310-73-2
研究领域: 环境科学 · 材料科学
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JOURNAL OF HAZARDOUS MATERIALS · 2021 · IF 10.588

Fungal laccase-triggered 17β-estradiol humification kinetics and mechanisms in the presence of humic precursors

Qingzhu Liu,Jie Liu,Dan Hong,Kai Sun,Shunyao Li,Abdul Latif,Xiongyuan Si,Youbin Si

Naturally-occurring phenolic acids (PAs) act as humic precursors that participate in the conversion behaviors and coupling pathways of steroidal estrogens (SEs) during laccase-triggered humification processes (L-THPs). Herein, the influences and mechanisms of PAs on Trametes versicolor laccase-evoked 17 β -estradiol (E2) conversion kinetics and humification routes were explored. Fungal laccase was fleet in converting > 99% of E2, and the calculated pseudo-first-order velocity constant and half-time values were respectively 0.039 min −1 and 17.906 min. PAs containing an O -dihydroxy moiety such as gallic acid and caffeic acid evidently hampered E2 humification owning to the yielded highly reactive O -quinones reversed E2 radicals by hydrogen transfer mechanism, implying that the inhibition effect was enormously dependent upon the number and position of the phenolic –OH present in humic precursors. Oligomers and polymers with carbon-carbon/oxygen links were tentatively found as E2 main humified species resulting from laccase-evoked successive oxidative-coupling. Note that PAs participating in the humification also encountered oxydehydrogenation, self-polymerization, and cross-binding to E2. Interestingly, the –COOH and –OCH 3 groups of PAs could be deprived in radical-caused self/co-polymerization. The generation of humified products not only circumvented the environmental risks of parent compounds but accelerated global carbon sequestration . To our knowledge, this is the first in-depth revelation of the humification pathways and related mechanisms of SEs with humic precursors in aquatic ecosystems by L-THPs.

研究领域: 环境科学 · 生物化学
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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY · 2024 · IF 5.9

CO2 sequestration by wet carbonated magnesium slag with high-content aragonite whiskers for improving cement performance as underground filling material

Boqiang Wu,Xiaodong Wang,Shibin Zhu,Yuehong Zhang,Junhao Ye,Haibo Zhang,Songhui Liu

Magnesium slag (MS) is an alkaline waste residue from magnesium smelting processes. This study aimed to utilize the magnesium oxide in MS and adopt MgCl 2 as the calcium carbonate crystal modifier to prepare high length-to-diameter ratio aragonite whiskers via wet carbonation , which can achieve high-value recovery of MS while capturing CO 2 and enhancing cement as underground filling material . The effects of MgCl 2 concentration on the carbonation process , composition, microstructure, and morphology were systematically investigated. With increasing MgCl 2 concentration, more aragonite was obtained, reaching 94.9 % at 0.5 M MgCl 2 . Notably, at 0.1 M MgCl 2 , high length-to-diameter ratio aragonite whiskers with 16 were achieved. Introducing 1 wt% MS carbonated at optimal 0.1 M MgCl 2 into cement increased the 3 d and 28 d compressive strengths by 17.8 % and 22 %, respectively. Moreover, an excellent CO 2 sequestration capacity of up to 20.33 g CO 2 per 100 g MS was obtained for the carbonated MS. Therefore, wet carbonated MS with high content aragonite whiskers is a promising method for MS high-value utilization while reducing cement usage and CO 2 emission, as well as improving cement performance as underground filling material.

CAS / MDL: 7791-18-6
研究领域: 材料科学 · 环境科学 · 矿业工程
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Heliyon · 2024 · IF 3.4

Clay mineral nanostructures regulate sequestration of organic carbon in typical fluvial sediments

Hongzhe Song,Zhifei Liu,Baozhi Lin,Yulong Zhao,Fernando P. Siringan,Chen-Feng You

The association between clay minerals and organic carbon is pivotal for understanding transport, burial, and preservation processes of sedimentary organic carbon. However, fine-scale microscopic studies are still limited in assessing the effect of diverse clay mineral structures and properties on organic carbon sequestration. In this study, we employed X-ray photoelectron spectroscopy, Fourier transform infrared spectroscopy, and transmission electron microscopy coupled with energy dispersive spectroscopy and electron energy loss spectroscopy analyses to investigate the nanoscale interaction between clay minerals and organic carbon of two typical fluvial sediment samples with contrasting clay mineral compositions and organic carbon origins. Sample from Taiwan shows abundant illite and chlorite with petrogenic organic carbon, while sample from Luzon has significant smectite with pedogenic organic carbon. We observed that the nanostructure of the clay minerals controls the distribution of organic carbon. In the Luzon sample, the organic carbon is tightly associated with smectite, occupying expandable interlayer spaces. In the Taiwan sample, however, the organic carbon is primarily confined on the surface and edge of illite. These findings offer valuable insights into the selective association of organic carbon with clay minerals and underscore the role of clay mineral nanolayer structures in governing the occurrence and preservation of organic carbon in sediments. A comprehensive understanding of these interactions is crucial for accurate assessments of carbon cycling and sequestration in the natural environment.

CAS / MDL: 7758-02-3
研究领域: 地质学 · 环境科学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2023 · IF 8.6

Dual-value utilization of calcium-silica slag: Sequestration of CO2 to recover high-purity vaterite with silica fertilizer as a by-product

Gangan Wang,Chaoyi Chen,Junqi Li,Xin Lin,Haonan Zheng

Calcium-silica slag (CSS) is a highly alkaline residue, rich in calcium, generated during the chemical pre-desilication process of medium- and low-grade bauxite. Mismanagement of CSS can result in detrimental environmental impacts. This study developed a novel method that combines CO 2 sequestration with CSS utilization, thereby achieving simultaneous dual-value enhancement of CSS and eliminating waste discharge. Under optimized Ca 2+ leaching and carbonation conditions, a remarkable Ca 2+ extraction efficiency of 96.93 % was attained, while the carbonation efficiency reached 99.37 %. Consequently, this process sequestered 301.7 kg of CO 2 per ton of CSS. The leaching process of Ca 2+ in NH 4 Ac solution was realized based on the unreacted shrinking core model, which accounts for internal diffusion and chemical reaction as factors influencing leaching. The resulting carbonated product exhibited outstanding characteristics: high-purity vaterite composed of 97.43 wt% CaCO 3 with a whiteness level of 95.2 %. By regulating the carbonation temperature, the crystal particulate size distribution of CaCO 3 was tailored to meet specific requirements for various applications. Furthermore, silicon content was enriched in the leaching residue, increasing the effective SiO 2 content from 25.2 wt% to 53.12 wt% and reducing the pH from 12.23 to 7.34, rendering it a suitable silica fertilizer for agricultural production.

研究领域: 环境科学 · 材料科学
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ENERGY & FUELS · 2024 · IF 5.2

CO2-Responsive Foam (CRF) for Mitigating CO2 Channeling in Heterogenous Reservoirs

Qi Gao,Xingguang Xu,Shuai Liu,Athumani Omari Mmbuji,Yunkun Wu

CO2 foam has been identified as having significant applications in carbon capture utilization and storage (CCUS). This is attributed to its proven capability to mitigate channeling during CO2 injection effectively; meanwhile, the majority of injected CO2 can be safely stored in reservoirs through geo-sequestration. However, the high injection pressure and poor foam stability severely affect the wide employment of CO2 foam flooding. In this study, comprehensive investigations on a novel CO2-responsive foam (CRF) with desirable injectivity and noticeable longevity are presented. This novel foam system employs lauryl ether sulfate sodium (LES) and diethylenetriamine (DETA) as foaming agents, and it exhibits notable reversible CO2-responsive properties. This property enables the fluid to transit between low and high-viscosity states, enhancing foam injection performance and reducing the injection pressure. CRF is less detrimental to reservoirs compared to conventional polymer-enhanced foam (PEF) due to its ability to switch between gel-forming and gel-breaking phases using CO2/N2. In addition, rheological tests demonstrate that CRF exhibits superior high shear tolerance compared to PEF. Moreover, CRF shows greater stability and higher salt resistance compared to PEF. At a NaCl concentration of 5 × 104 mg/L, the half-life of CRF (152 min) was nearly 13 times longer than that of PEF (11 min). It is noted that CRF exhibits a higher resistance factor in high-permeability cores compared to low-permeability cores, indicating its outstanding capacity to block the channels and mitigate CO2 breakthrough. The results of the enhanced oil recovery (EOR) experiments indicated that CRF is capable of displacing more oil than PEF in fractured cores with identical experimental conditions. It is believed that CRF may be applied as a viable CCUS technique and may enlighten investigations on novel CCUS strategies.

研究领域: 石油工程 · 环境科学
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SCIENCE OF THE TOTAL ENVIRONMENT · 2023 · IF 9.8

CO2 sequestration and CaCO3 recovery with steel slag by a novel two-step leaching and carbonation method

Can Cheng,Wenjun Huang,Haomiao Xu,Zhisong Liu,Xianwei Li,Hongzhi Shi,Yongmei Yu,Zan Qu,Naiqiang Yan

The steel smelting process produces extensive CO 2 and Ca-containing steel slag (SS). Meanwhile, the low value utilization of steel slag results in the loss of Ca resources. CO 2 sequestration utilizing SS can reduce carbon emissions while achieving Ca circulation. However, conventional SS carbon sequestration methods suffer from slow reaction rates, finite Ca usage efficiency, and difficulty separating the CaCO 3 product from SS. Herein, an innovative two-step leaching (TSL) and carbonation method was presented based on the variations in leaching efficiency of activated Ca under different conditions, aiming at efficient leaching, carbon sequestration, and high-value reuse of SS. This method employed two NH 4 Cl solutions in sequence for two leaching operations on SS, allowing the Ca leaching rate to be effectively increased. According to the findings, TSL could increase the activated Ca leaching rate by 26.9 % and achieve 223.15 kg CO 2 /t SS sequestration compared to the conventional one-step leaching (CSL) method. If part of the CaCO 3 is recovered as a slagging agent, about 34.1 % of the exogenous Ca introduction could be saved. In addition, the CO 2 sequestration of TSL did not significantly decrease after 8 cycles. This work proposes a strategy that has the potential for recycling SS and reducing carbon emissions.

研究领域: 环境科学 · 材料科学 · 化学工程
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Journal of Environmental Sciences · 2023 · IF 6.9

Bipolar membrane electrodialysis integrated with in-situ CO2 absorption for simulated seawater concentrate utilization, carbon storage and production of sodium carbonate

Jingtao Bi,Tianyi Chen,Yue Xie,Ruochen Shen,Bin Li,Mengmeng Sun,Xiaofu Guo,Yingying Zhao

In the context of carbon capture, utilization, and storage, the high-value utilization of carbon storage presents a significant challenge. To address this challenge, this study employed the bipolar membrane electrodialysis integrated with carbon utilization technology to prepare Na 2 CO 3 products using simulated seawater concentrate, achieving simultaneous saline wastewater utilization, carbon storage and high-value production of Na 2 CO 3 . The effects of various factors, including concentration of simulated seawater concentrate, current density, CO 2 aeration rate, and circulating flow rate of alkali chamber, on the quality of Na 2 CO 3 product, carbon sequestration rate, and energy consumption were investigated. Under the optimal condition, the CO 3 2– concentration in the alkaline chamber reached a maximum of 0.817 mol/L with 98 mol% purity. The resulting carbon fixation rate was 70.50%, with energy consumption for carbon sequestration and product production of 5.7 kWhr/m 3 CO 2 and 1237.8 kWhr/ton Na 2 CO 3 , respectively. This coupling design provides a triple-win outcome promoting waste reduction and efficient utilization of resources.

研究领域: 环境科学 · 化学工程 · 碳捕集与利用
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CARBOHYDRATE POLYMERS · 2024 · IF 10.7

Continuously enhanced versatile nanocellulose films enabled by sustaining CO2 capture and in-situ calcification

Wenjing Li,Jilun Guan,Huayang Fang,Yuheng Jiang,Yu Zhong,Shaohong Shi,Fangchao Cheng

Cellulose possesses numerous favorable peculiarities to replace petroleum-based materials. Nevertheless, the extremely high hygroscopicity of cellulose severely degrades their mechanical performance, which is a major obstacle to the production of high-strength, multi-functional cellulose-based materials. In this work, a simple strategy was proposed to fabricate durable versatile nanocellulose films based on sustaining CO 2 capture and in-situ calcification. In this strategy, Ca(OH) 2 was in-situ formed on the films by Ca 2+ crosslinking and subsequent introduction of OH − , which endowed the films with high mechanical strength and carbon sequestration ability. The following CO 2 absorption process continuously improved the water resistance and durability of the films, and enabled them to maintain excellent mechanical properties and promising light management ability. After a 30-day CO 2 absorption process, the water contact angle of the films can be increased from 43° to 79°, and the weight gain rate of the films in a 30 h water-absorption process can be sharply decreased from 331.2 % to 52.2 %. The films could maintain a high tensile strength of 340 MPa, and result in a CO 2 absorption rate of 3.5 mmol/g cellulose after 30 days. In this study, the improvement of durability and carbon sequestration of nanocellulose films was achieved by a simple and effective method.

研究领域: 材料科学 · 环境科学 · 生物学
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CHEMICAL ENGINEERING JOURNAL · 2017 · IF 6.216

Accelerated mineral carbonation curing of cement paste for CO2 sequestration and enhanced properties of blended calcium silicate

Tao Wang,Hao Huang,Xutao Hu,Mengxiang Fang,Zhongyang Luo,Ruonan Guo

The mineral carbonation (MC) curing of cement-based materials could be employed to obtain both CO 2 sequestration and accelerated strength gain. But there is still absence of understanding on the gas-solid reaction kinetics and mechanisms. This study aims to improve the understanding of gas-solid reaction between CO 2 and cement-based materials during the MC curing, and evaluate the feasibility of blending calcium silicate (CS) as intensified addition. Based on the accelerated carbonation experiments, the impact of different factors (pressure, temperature and water-to-binder rate) on the reaction rate and the CO 2 uptake were systematically investigated. The MC curing showed significant diffusion-controlled kinetics and the reaction gradually turned into the stable product-layer diffusion controlling process. The evolution process of kinetics indicated the increasingly dense structure of cement matrix, as verified by SEM analysis. The blended CS was found to significantly enhance the reaction rate and CO 2 uptake capacity, accompanied with the intensified carbonation conversion of cement components. The increased Klinkenberg permeability of blended CS paste after MC curing demonstrated the diluted effect of CS. In terms of the practical feasibility, MC curing also contributed remarkably to the compressive performance improvement of cement paste with blended CS.

CAS / MDL: 75-15-0
研究领域: 材料科学 · 环境科学
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