INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2025
·
IF 3.9
Zhiyang Yu,Yuqi Shao,Wenyao Li,Yongzhuo Liu
Integrated CO2 capture and conversion (ICCC), which simultaneously achieves CO2 enrichment and in situ conversion, represents a promising strategy for reducing CO2 emissions. Dual-function materials (DFMs) that exhibit stable and highly efficient adsorption and catalytic conversion properties are essential to the success of this strategy. In this study, we developed novel Mo/Fe-doped CaO-based DFMs for the integrated CO2 capture and reverse water–gas shift (ICCC–RWGS) process. The synthesized DFMs was evaluated through adsorption–conversion cyclic experiments in a fixed-bed reactor, complemented by X-ray diffraction (XRD), Brunauer–Emmett–Teller (BET), scanning electron microscopy (SEM) mapping, and X-ray photoelectron spectroscopy (XPS) characterizations. The results indicate that the generated composites with a specialized structure not only provide stable support for CaO but also regulate the RWGS process. Specifically, the formation of Ca2Fe2O5 facilitates the hydrogenation of CaCO3 via redox reactions, while the generation of CaMoO4 and Ca2FeMoO6 alleviates both the volume-change effects of CaO caused by CO2 adsorption–hydrogenation cycles and the carbon deposition side reactions caused by Fe. DFMs with a Mo/Fe mass ratio of 1:9 exhibited a CO2 capture capacity of 14.8 mmol/g DFM, a CO yield of 11.4 mmol/g DFM, and good cyclic properties at 650 °C, making it a promising DFM for ICCC–RWGS. In conclusion, the utilization of superstructures with superior redox reactivity and structural stability, such as perovskite and spinel, offers valuable insights into the design of DFMs for ICCC.
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Chemical Science
·
2025
·
IF 7.4
Lei Xu,Qun Xu,Buxing Han
The advancement of nanotechnology has enabled magnetic nanomaterials to exhibit remarkable potential and application value in medicine, transportation, information storage, and spintronics owing to their unique physicochemical properties. In this study, supercritical carbon dioxide (SC CO2) was used to successfully induce room-temperature ferromagnetism in CaSnO3 without magnetic element doping, achieving a maximum saturation magnetization of 0.0727 emu g−1 at 16 MPa. The SC CO2 treatment introduced lattice-scale defects, releasing residual force within distorted SnO6 octahedra, which led to the suppression of structural distortion and drove a structural phase transition from orthorhombic to cubic. Additionally, the enhanced symmetry was accompanied by anisotropic lattice expansion and tensile strain, which thermodynamically lowered the oxygen vacancy formation energy, thereby kinetically driving the creation of more defects. This disrupted the intrinsic antiferromagnetic order and significantly enhanced ferromagnetism. This work elucidates a defect-strain synergy mechanism for tuning material magnetic order, distinguishing it from conventional stoichiometric doping strategies and highlighting the critical role of SC CO2 in material modification.
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CHEMICAL ENGINEERING SCIENCE
·
2025
·
IF 4.3
Chang Liu,Xin Meng,Feng Hou,Fengming Ma,Yanchen Li,Ling Yin,Guoxiang Yue,Dongfang Guo,Hongwei Niu,Shiwang Gao,Huanjun Wang
Carbon dioxide (CO 2 ) chemisorption employing biphasic solvents is recognized as a method with substantial application potential. Nevertheless, under conditions of burning high-sulfur fuels or rapid load changes, SO 2 in the flue gas poses challenges to the stability and economic operation of biphasic CO 2 capture system. To tackle this, the impact of residual SO 2 on CO 2 capture performance was systematically investigated in a lab‑scale continuous absorption–desorption set-up using novel biphasic solvent. The system achieved steady CO 2 capture efficiencies of 97.8 % and 94.8 % over 20 days without SO 2 . In the presence of SO 2 , CO 2 capture efficiency declined from >90 % in the first 10 days to below 80 % after 13 days and 70 % after 17 days, owing to irreversible reactions between SO 2 and amine, pH drop, and amine loss. CO 2 loading and circulation capacity similarly decreased, while CO 2 desorption duty rose from 2.51 to over 5.0 GJ/t CO 2 , driven by increased solvent flow and amine degradation catalyzed by SO 4 2− . DFT calculations indicated that the dissolution of SO 2 formed SO 3 2− /SO 4 2− , which enhanced the hydration of CO 2 . However, SO 2 preferentially reacted with amines, acidifying the interface and hindering CO 2 absorption. Quantitative 13 C NMR indicated that the oxyanion produced by the dissolution of SO 2 reduced the concentrations of bicarbonates and carbonates in the rich phase. A mechanistic model based on film theory was proposed, delineating gas‑phase diffusion, liquid‑phase competition, and catalytic promotion by oxyanions. These findings guided recommendations for pretreatment and solvent‑management strategies to ensure stable biphasic CO 2 capture under real flue gas conditions.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2025
·
IF 6.3
Furong Tao,Yuning Zhang,Yunqi Miao,Ruirui Qi,Zizheng Lv,Haimei Xu,Zhichao Miao,Xingxiang Ji
Electrocatalytic CO 2 reduction (ECR) to high-value formic acid is an important approach for realizing carbon resource recycling and renewable energy storage. A key challenge in this process is the development of highly efficient and stable catalysts. In this work, three types of mesoporous catalysts, In 2 O 3 -ZrO 2 , SnO 2 -ZrO 2 , and Bi 2 O 3 -ZrO 2 , were prepared through a one-step method. The influence of type and existing state of active components on catalytic performance was researched in depth. These results indicate that the introduced active components exhibit a strong interaction with ZrO 2 support and exist as a highly dispersed state in the support. Among the prepared catalysts, the In 2 O 3 -ZrO 2 demonstrates superior activity and stability, achieving a formate Faraday efficiency of 90 % and a current density of 110 mA cm −2 at −1.17 V vs. RHE, while maintaining stable performance over an 80 h long-term ECR test. In addition, the mesoporous material with high specific surface area provides a greater number of active sites, thus contributing to the enhanced catalytic performance. This study provides a new catalyst synthesis strategy for ECR to formate and offers guidance for preparing high-efficiency catalysts.
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FUEL
·
2025
·
IF 7.5
Ziwen Hao,Yabin Li,Yutong Pan,Xiaoyu Han,Qiang Wang,Maoshuai Li,Yue Wang,Xinbin Ma
Interaction between metal species and support affects the structural and electronic properties of metal species, thus changing the catalytic behaviour. This work demonstrates regulation of support size is an effective way to optimise the metal-support interaction over Ni/CeO 2 -cube. Smaller ceria cubes promoted formation of smaller Ni particle sizes with higher dispersion, generating stronger interaction between Ni and CeO 2 , and consequently higher turnover frequency for CO 2 methanation. The interaction in Ni/CeO 2 with the smallest ceria size (average ca. 5 nm) provides stronger CO 2 and H 2 adsorption capacity, facilitating the CO 2 methanation with over 99 % CH 4 selectivity at 548–573 K, delivering a CO 2 conversion rate of 327.9 mol CO2 mol Ni -1 h −1 , which is 1.9 and 14.0 times than that of the 12 nm and 20 nm counterparts at 573 K, respectively. In-situ FTIR spectroscopic analysis demonstrates the surface reaction proceeds via a formate pathway, and smaller CeO 2 -cube supported Ni facilitates conversion of carbonate/bicarbonate intermediates to formate species. The metal-support interaction aroused from controlled support size provides a new way to design high-performance methanation catalyst.
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APPLIED SURFACE SCIENCE
·
2025
·
IF 6.9
Yuewen Chen,Tao Zheng,Hai Liu,Weidong Xie,Jiali Huang,Yimin Wang,Xiya Zhang,Zhen Yuan,Zhile Xiong
The electrocatalytic reduction of CO 2 to CO represents an important approach for carbon resource utilization. However, most existing catalysts still suffer from low activity and poor selectivity. In this work, a novel “domain-confined interface” synergistic catalytic system was constructed by integrating ionic liquid [BMIM][BF 4 ] with zeolitic imidazolate framework-8 (ZIF-8) to enhance the CO 2 reduction reaction (CO 2 RR) performance. The high specific surface area and microporous structure of ZIF-8 provide an ideal platform for CO 2 adsorption and activation, while [BMIM][BF 4 ] improves the local microenvironment of the catalytic interface, thereby boosting the catalytic activity. Experimental results indicate that the incorporation of the ionic liquid significantly enhances the CO 2 RR performance of ZIF-8 at low potentials. The Faradaic efficiency for CO (FE CO ) increases from 38.98 % to 75.25 % at −0.8 V versus the reversible hydrogen electrode (RHE). Moreover, at the optimal potential of −1.2 V (vs. RHE), FE CO reaches 96 % and remains stable during an 8-hour durability test, outperforming most reported ZIF-8-based catalysts. This work may provide useful insights for the design of efficient CO 2 RR electrocatalysts.
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INORGANIC CHEMISTRY COMMUNICATIONS
·
2025
·
IF 5.4
Xingxing Zhao,Yudong Ding,Lijiao Ma,Xun Zhu,Hong Wang,Min Cheng,Qiang Liao
Porous liquids are promising absorbents for CO 2 capture due to porosity and liquidity. In this paper, three amines, TEPA, PEI, and MEA, were used to reinforce CO 2 capture in type III porous liquids, and the influences of these amines on the CO 2 uptake of the porous liquids were discussed. First, determining the optimal TEPA, PEI, and MEA loadings were 30 wt%, 30 wt%, and 50 wt%, respectively. Then, the amine-modified type III porous liquids, TEPA@ZIF-8/[EMIm]/[NTf 2 ], PEI@ZIF-8/[EMIm]/[NTf 2 ], and MEA@ZIF-8/[EMIm]/[NTf 2 ] were prepared. The effects of different parameters on the CO 2 absorption characteristics were systematically investigated. It was found that amines-modification could significantly reinforce CO 2 absorption of type III porous liquids at low CO 2 partial pressures. The CO 2 uptake capacity of 5-30TEPA@ZIF-8/[EMIm][NTf 2 ], 5-30PEI@ZIF-8/[EMIm][NTf 2 ], 5-50MEA@ ZIF-8/[EMIm][NTf 2 ] was 4.43, 2.28, and 3.96 times higher and the corresponding absorption rates were 8.45, 2.25, and 26.3 times higher than that of 5-ZIF-8/[EMIm][NTf 2 ]. The CO 2 absorption kinetic properties were revealed, and the results showed the fractional-order kinetic model best fitted the CO 2 absorption process, suggesting the CO 2 absorption coupled with the CO 2 diffusion inside the main units and the chemical reaction at the active sites. Finally, the cyclic regeneration performance results displayed that TEPA@ZIF-8/[EMIm][NTf 2 ] exhibited a good cyclic regeneration performance and has the potential for CO 2 capture.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Jinpeng Zhai,Zhenjiang Wang,Jia Ouyang,Beichen Xue,Chao Liu,Rui Xiao
Sewage sludge (SS), as a common solid waste with large production and rich organic nitrogen, has the potential to synthesize N-doped carbon (N-C) for CO 2 adsorption. In this paper, A novel synthesis method of N-C CO 2 adsorbent from SS by structural regulation of glucose (Glc) and further activating with K 2 CO 3 was proposed. Besides, the influence mechanism of N-doping form and content on CO 2 absorption capacity of N-C was studied by density functional theory calculations (DFT). Results showed that Glc had the effect of promoting the formation of internal mesoporous structure and adjusting pyrrole-N (N-5) structure into quaternary-N (N-Q) structure. The N-C prepared with feedstock mixing sludge, Glc and K 2 CO 3 powder (mass ratio of SS/Glc/K 2 CO 3 = 3:1:4) at 800 °C showed the highest CO 2 adsorption capacity (3.00 mmol/g at 25 °C and 1 bar) and superior CO 2 selectivity for CO 2 /CO/CH 4 under continuous flow. Theoretical calculations identified a nitrogen-doping threshold effect, where elevated nitrogen content strengthened pyridine-N (N-6) induction effects to enhance localized polarity for CO 2 adsorption. Conversely, lower doping levels amplify conjugation effects via N-5 prevalence, significantly improving adsorption capacity. This dual mechanism demonstrates that N-6 configurations optimize local polarity at high doping ratios, while N-5 architectures maximize electron delocalization efficiency at reduced nitrogen concentrations.
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MOLECULES
·
2025
·Vol. 30
·期 8
·1804
·
IF 4.6
Wentao Xiang,Zhenzhen Yu,Renwu Gao,Zhichao Yi,Kun Gong,Kangqiang Lu,Weiya Huang,Changlin Yu,Zeshu Zhang,Man Zhou,Kai Yang
Rapid charge separation and transfer is the key scientific problem in photocatalysis. The construction of S-scheme heterojunction is one of the effective strategies to promote charge separation and maintain the strong redox properties. Herein, the NiO, K0.2WO3, and NiWO4ternary double S-scheme K0.2WO3/NiO/NiWO4heterojunction (W/NiO) was created by a one-step molten salt method. Ultraviolet-visible (UV-Vis) diffuse reflectance spectra, photoluminescence (PL) spectra, photoelectrochemistry tests, and other analyses revealed that the double S-scheme heterostructure broadened the spectral response range of NiO and promoted its separation of photocarriers. Compared with pristine NiO, the modified double S-scheme heterojunction enhanced the surface adsorption of water molecules and the accumulation of intermediate product of HCOO−, and optimized the CO2reduction system, realizing the improved CO yield of 373 μmol·g−1·h−1in Ru(byp)32+/ethanolamine of CO2reduction system. This study indicates that double S-scheme heterojunction could facilitate efficient photogenerated charge transfer and separation, thereby achieving high activity and selectivity for CO2photoreduction. Our work provides a reference for the one-step construction of double S-scheme heterojunction.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Dongdong Zhang,Jiang Zhong,Linjie Tong,Peng Chen,Xingan Jiang,Lin Wang,Xiaoqiang Zhan,Hongli Yang,Hongxian Zhu,Yong Luo,Weiyou Yang
Single-atom catalysts (SACs) show great potential in enhancing CO 2 photoreduction activity, thanks to their exceptional atomic efficiency and outstanding catalytic properties. However, the high surface energy of SACs presents a significant challenge, as the single atoms often tend to be aggregated during the synthesis and catalytic processes, thus making them be difficult for efficient and sustainable performance. Herein, we report a strategy to stabilize SACs on photocatalytic materials enabled by creating oxygen vacancy defects on the matrix surface, which allow the single-atom platinum (Pt) uniformly and solidly anchored on BiOBr nanosheets (NSs). The as-synthesized Pt-BiOBr-V O achieves a dramatic CO 2 photoreduction activity with a CO production rate of 93.5 μmol·g −1 ·h −1 and 75 % selectivity, outperforming those of most BiOBr-based photocatalysts ever reported. The overall enhanced catalytic behaviors are mainly attributed to the synergistic effect between the Pt single atoms and V O , which optimizes the electronic structure of BiOBr with improved charge transfer and extended lifetime of photogenerated carriers. Moreover, the created oxygen vacancies could act as the electron absorption centers, thus accelerating the activation of CO 2 and the formation of intermediates. The present work provides new insights on rationally designing highly efficient and stable photocatalysts based on defect engineering for developing sustainable green energy.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Xiaoyan Zhang,Wenkang Ni,Peihang He,Zhijie Wang,Ke Wang,Zizhong Zhang,Wenxin Dai,Xianzhi Fu
Photocatalytic CO 2 reduction comprises two coupled half-reactions: CO 2 reduction and H 2 O oxidation. Efficient coupling of these reactions maximizes the utilization of photogenerated electrons and holes, enhancing CO 2 conversion and product selectivity. In this study, sulfur-deficient V S -Zn 3 In 2 S 6 (V S -ZIS) catalysts were synthesized via an ethylene glycol solvothermal method, followed by anchoring Fe single-atom sites (Fe/V S -ZIS) to facilitate CO 2 photoreduction using H 2 O as proton source. The 1 %Fe/V S -ZIS exhibited exceptional performance, with a CO production rate of 88.6 μmol·g −1 ·h −1 and 97 % selectivity. Experimental and DFT results revealed that V S functioned as reductive sites to strengthen CO 2 adsorption and activation, while Fe single atoms (SAs) served as oxidative sites to facilitate H 2 O dissociation for proton supply. Fe SAs also induced spin polarization to enhance IEF, thereby suppressing photogenerated charges recombination at redox sites. Meanwhile, Fe SAs reduced COOH* formation energy barrier and lowered CO desorption temperature, improving CO selectivity. The constructed dual active sites synergistically enhanced the overall photocatalytic CO 2 reduction performance. This work offers new technical pathways for designing redox dual-active sites to boost the overall photocatalytic CO 2 reduction efficiency.
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ACS Omega
·
2025
·
IF 4.3
Yongqi Sun,Fujun Sheng,Guangyu Sun,Jiaxuan Wang,Lei Shi
Supercritical CO2 (scCO2) extraction exerts a significant effect on the physicochemical characteristics of crude oil. This work focuses on the role that waxes and asphaltenes played in the scCO2 extraction effect. The extraction rate, hydrocarbon composition, wax precipitation characteristics, conductivity, and centrifugal stability are quantitatively characterized. It is found that the extraction rate of model oil without paraffin wax is the highest after scCO2 treatment, approximately 18.3%. When the paraffin wax content is enlarged from 5.0 to 15.0 wt %, the extraction rate decreases from 16.7% to 11.7%. It is indicated that the presence of wax inhibits the extraction effect of scCO2. In addition, with further addition of asphaltenes, the extraction rate increases and then decreases. This manifests that the addition of asphaltene promotes the extraction effect of scCO2, while the combined effect of waxes and asphaltenes inhibits the extraction effect with the further increase of the asphaltene concentration. Considering the wax precipitation characteristics, the wax appearance temperature (WAT) and wax precipitation amount (WPA) are both increased after scCO2 treatment. With the addition of asphaltene, the WAT and WPA of model oil are both decreased. As for wax crystal morphology, the wax crystals in paraffin wax oil become finer after the treatment, and the amount of wax crystals precipitated increases. Lastly, after scCO2 treatment, the conductivity and absorbance of model oil containing asphaltene decrease, while the light transmittance increases, due to the formation of asphaltene aggregates under scCO2.
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