CHEMICAL ENGINEERING JOURNAL
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2024
·
IF 13.3
Lixin Song,Guobin Liu,Zhenping Qu
CO 2 hydrogenation to methanol and/or dimethyl ether (DME) holds promise for mitigating greenhouse gas effects and addressing energy scarcity. However, the relationship between product selectivity and the collective nature of the catalysts remains ambiguous due to the intricate reaction network. Here, a series of Cu/Zn x Al y O z catalysts with different surface properties have been engineered by manipulating the Zn/Al ratio to achieve product controllability for CO 2 hydrogenation. The results unveil the pivotal role of the H 2 dissociation capability in governing CO 2 conversion, which is regulated by the concentration of Cu 0 species. Furthermore, the number of surface hydroxyl groups, the proportion of moderately strong basic sites and moderately strong acidic sites show desirable linear correlations with the selectivity of CO, CH 3 OH, and DME, respectively. Importantly, the ZnAl 2 O 4 -Al 2 O 3 or Cu-ZnAl 2 O 4 -Al 2 O 3 interface notably enhances moderately strong acidic sites, aiding methanol dehydration to DME. This work offers a comprehensive guide to the rational design of catalysts for oriented product synthesis from CO 2 hydrogenation.
研究领域:
催化化学
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能源化学
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材料科学
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DOI
高影响因子
Carbon Letters
·
2023
·Vol. 33
·期 5
·1395-1406
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IF 4.5
Chen Zhangjing,Li Liangliang,Cheng Gang
Photocatalytic CO 2 reduction is a promising approach for reducing CO 2 emissions and achieving the goal of carbon neutrality. In this work, selectively coupling Cu(OH) 2 and CuO with amine-modified brookite TiO 2 (NH 2 –B–TiO 2 ) has been achieved by a simple precipitation method. The results show that CuO is better than Cu(OH) 2 as a co-catalyst to enhance the CO 2 photoreduction capability of NH 2 –B–TiO 2 . The highest rates of CO 2 conversion to CH 4 and CO of NH 2 –B–TiO 2 –CuO composite reach 6.05 and 3.25 μmol h −1 g −1 , respectively, which is higher than 8 times the yield of CH 4 of NH 2 –B–TiO 2 . It is proposed that the NH 2 –B–TiO 2 –CuO composite offers an effective charge transfer through the formation of a p–n junction between NH 2 –B–TiO 2 and CuO interfaces, while in the NH 2 –B–TiO 2 –Cu(OH) 2 composite, the Cu(OH) 2 dominantly serves as an electron sink to capture photo-induced electrons, promoting photo-induced carrier separation. This work provides an ingenious synthetic method for selectively anchoring Cu(OH) 2 and CuO on semiconductors with different charge transfer routes for an efficient CO 2 photoreduction. Graphical abstract
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
高影响因子
JOURNAL OF MOLECULAR LIQUIDS
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2024
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IF 5.3
Wentao Zheng,Jialing Chen,Yujiao Jia,Nengqi Sun,Shiping Wang,Xianku Wu,Xuehua Zhang
A series of 1,8-Diazabicyclo[5.4.0]undec-7-ene (DBU)/N-heterocyclic DESs aqueous solutions were designed and synthesized as CO 2 capture agents. They showed excellent performance in absorption capacity, especially for the low-pressure CO 2 . The CO 2 loads in the absorbents were higher than 1.0 mol/mol when the pressure was just 0.1 bar. Through a combination of 13 C NMR spectra, FT-IR spectra and absorption experiments, a novel absorption mechanism was proposed. It was the shuttling role of the carbamate generated from CO 2 and nitrogen heterocycles, along with the synergistic roles of the DBU and water, that caused the high absorption capacity of the DBU/N-heterocyclic DESs for CO 2 . Meanwhile, the thermodynamic parameters, the activation energy and the regeneration efficiency were all measured to estimate the absorption performance of the DBU/N-heterocyclic DESs aqueous solutions for low-concentration CO 2 .
研究领域:
化学
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环境科学
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产品关联
DOI
高影响因子
Materials Chemistry Frontiers
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2025
·
IF 6.4
Yapeng Dong,Yuning Liang,Bo Gao,Qun Xu
Exploring advanced technology to obtain quantum materials presenting novel and unexpected electronic states upon proper manipulation is an important research endeavor. Usually, plastic deformation can lead to some amount of disruption that can result in new physical phenomena and fascinating structures. However, how to realize efficient plasticization and manipulation to obtain irreversible variation in such materials, especially those presenting quantum material behavior, is a great challenge. Herein, we show that upon plastic deformation induced by supercritical CO2 (SC CO2) on SrZrO3, typically at a pressure of 16 MPa, SrZrO3 experiences a transition from a bulk material to a two-dimensional (2D) structure. More importantly, it can be observed that the octahedral rotation of ZrO6 is suppressed. Furthermore, plastic deformation frequently induces magnetism in SrZrO3. Via polarization characterization, SrZrO3 displays multiferroic characteristics, exhibiting a considerable enhancement in the saturation magnetisation strength and polarization strength. At room temperature, SrZrO3 exhibits a saturated magnetisation of 0.1280 emu g−1, accompanied by a polarization of 0.27 μC cm−2. Therefore, this work demonstrates that plastically deformed SrTiO3 induced by SC CO2 can successfully transition into a quantum multiferroic material. These results establish a new method toward plastic deformation for the manipulation of the electronic properties of quantum materials.
研究领域:
材料科学
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凝聚态物理
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量子物理
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DOI
高影响因子
Chemical Science
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2018
·Vol. 9
·期 14
·3426-3437
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IF 9.063
Xinyu Li,Zhi-Jian Zhao,Liang Zeng,Jiubing Zhao,Hao Tian,Sai Chen,Kang Li,Sier Sang,Jinlong Gong
La2O3 exhibits good performance for various catalytic applications, such as oxidative coupling of methane (OCM) and dry reforming of methane (DRM), during which coke formation may lead to the deactivation of catalysts. Typically, the reaction between CO2 adsorbed on La2O3 and coke is the rate-determining step of the coke elimination process. This paper describes the influence of Ce addition on the CO2 adsorption and activation over La2O3. Combined with in situ and ex situ characterization and density functional theory (DFT) calculation, we show that Ce addition promotes the formation of bidentate carbonate on La2O3via tuning CO2 adsorption energy. In addition, Ce addition adjusts the ratio of bidentate/monodentate carbonate, and affects the ratio of hexagonal/monoclinic La2O2CO3 on the binary oxides. DRM is used as a probe reaction to examine the coke elimination performance of Ce–La binary oxide. It is found that when the Ce/La ratio reaches the optimal value (0.15), Ce–La binary oxide has the highest CO2 adsorption energy and predominantly promotes the formation of bidentate carbonate, and hence possesses the highest basicity above 700 °C and finally exhibits the best coke elimination performance.
研究领域:
催化化学
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材料科学
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DOI
PubMed
高影响因子
NANO
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2024
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IF 1
Xuecong Ma,Linlin Geng,Yu Li,Jianwen Wei,Lei Liao,Dunqiu Wang
Micro/mesoporous materials are low-cost functional materials with the potential for CO 2 adsorption. Modifying micro/mesoporous materials is significant for enhancing CO 2 adsorption and their high-value utilization. Herein, the micro/mesoporous material of composite molecular sieve ZSM-5/MCM-48 (ZM) was synthesized by a two-step crystallization method using cetyltrimethylammonium bromide as a template, tetraethyl orthosilicate as a silicon source and ZSM-5 seed as part of silicon aluminum source. Tetraethylenepentamine (TEPA) and polyethyleneimine (PEI) were used as impregnation modifiers to modify ZM with amine groups. The results showed that with the increase of amine loadings, both ZM-T60 (Impregnated with TEPA) and ZM-P60 (Impregnated with PEI) functionalized adsorbents exhibited the best adsorption capacities of 4 . 9 7 mmol ⋅ g − 1 and 3 . 2 8 mmol ⋅ g − 1 at 60, respectively, when the loading of ZM sample was 60%. The adsorption kinetic analysis showed that the adsorption of CO 2 by ZM-T60 and ZM-P60 was a chemisorption-dominated process accompanied by physical adsorption. After 10 adsorption/desorption cycles, the CO 2 adsorption capacity of ZM-T60 and ZM-P60 decreased by 8.7% and 2.6%, respectively. This work demonstrates that impregnation modification of the composite molecular sieve to achieve efficient CO 2 adsorption has practical application significance.
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
高影响因子
Journal of Materials Chemistry A
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2025
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IF 9.5
Yi Chen,Weilin Shi,Claudia Li,Kang Hui Lim,Xueqian Wang,Langlang Wang,Ping Ning,Yixing Ma,Sibudjing Kawi
Global warming, driven by rising levels of CO2 in the atmosphere, is an environmental predicament confronted by humanity. Plasma catalytic decomposition of carbon dioxide into carbon monoxide is a practical approach to mitigate this challenge, which can be a crucial step in carbon recycling. Metal selenides are promising candidates owing to their abundant reserves and outstanding electron transfer properties, making them highly active in chemical reactions. In this study, the morphology of AlO(OH) and the dispersion of Cu2−xSe were optimized by hydrothermal synthesis temperature. Specifically, the Cu2−xSe-Al-180 catalyst, prepared at a hydrothermal temperature of 180 °C, formed AlO(OH) with good crystallinity and a nanoscale thin-sheet structure, with Cu2−xSe uniformly distributed on the AlO(OH) support. The reaction of CO2 decomposition to CO production by integrating Cu2−xSe-Al-180 with dielectric barrier discharge (DBD) plasma led to a CO2 conversion of up to 28.07% at a specific input energy (SIE) of 58.07 kJ L−1. The excellent CO2 adsorption properties of AlO(OH) and Cu2Se reduce the activation energy barrier of the reaction, and Cu2Se further promotes the excited activation of CO2 in the plasma. These findings offer valuable insights for the development and design of catalysts in the field of plasma catalysis and highlight the potential of CuSe-based materials in CO2 reduction technologies.
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
Catalysts
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2025
·Vol. 15
·期 1
·95
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IF 4
Jinghong Fang,Min Wang,Xiaotong Yang,Qiong Sun,Liyan Yu
In this study, a novel Z-scheme heterojunction photocatalyst was developed by integrating g-C3N4nanoplates into ZnIn2S4microspheres. X-ray photoelectron spectroscopy analysis revealed a directional electron transfer from g-C3N4to ZnIn2S4upon heterojunction formation. Under irradiation, electrochemical tests and electron paramagnetic resonance spectroscopy demonstrated significantly enhanced charge generation and separation efficiencies in the ZnIn2S4/g-C3N4composite, accompanied by reduced charge transfer resistance. In photocatalytic CO2reduction, the ZnIn2S4/g-C3N4composite achieved the highest CO yield, 1.92 and 5.83 times higher than those of pristine g-C3N4and ZnIn2S4, respectively, with a notable CO selectivity of 91.3% compared to H2(8.7%). The Z-scheme heterojunction mechanism, confirmed in this work, effectively preserved the strong redox capabilities of the photoinduced charge carriers, leading to superior photocatalytic performance and excellent long-term stability. This study offers valuable insights into the design and development of g-C3N4-based heterojunctions for efficient solar-driven CO2reduction.
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
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Jinsong Shi,Jianguo Xu,Hongmin Cui,Nanfu Yan,Runhan Yan,Yaqing Weng
Porous carbon is a very promising type of CO 2 adsorbent due to its excellent stability, low cost, and tunable physicochemical properties. In the current work, N-doped hierarchically porous carbon was synthesized with the assistance of NaCl template and KHCO 3 activation. A series of carbons with three dimensional and interconnected micro- meso -macroporous structure were successfully prepared. Effects of synthesis conditions on textural properties and N-doping were analyzed and discussed with details. The carbons also exhibited high surface area (725–2423 m 2 /g) and N content (1.49–7.93 wt%). CO 2 adsorption properties were studied with a combined experimental and theoretical approach. At 25 °C and 1 bar, the carbons exhibited CO 2 uptake up to 4.22 mmol/g and CO 2 /N 2 selectivity up to 25.6. Grand canonical Monte Carlo (GCMC) simulation was employed to further elucidate the different roles played by N-doping and textural properties during CO 2 adsorption. Effects of various N-functionalities located in pores with different sizes on CO 2 adsorption were thus revealed. The present study presents a novel strategy for controlled synthesis of porous carbons, and provides helpful insights into their CO 2 adsorption behaviors.
研究领域:
材料科学
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环境科学
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产品关联
DOI
高影响因子
Surfaces and Interfaces
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2025
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IF 6.3
Pengcheng Xiang,Lili Wang,Qin Geng,Changyan Guo,Hongtao Xie,Yizhao Li,Yangyang Yu,Jide Wang
Structural design of semiconductor photocatalysts plays an important role in promoting light absorption, molecular activation, and charge separation in the CO 2 reduction reaction, which is beneficial for improving photocatalytic activity. In this paper, a simple photodeposition strategy was employed to load Cu onto Bi 2 O 2 SO 4 and form a Cu-Bi alloy. Under simulated sunlight conditions, the optimal catalyst demonstrates impressive photocatalytic activity and selectivity for CO 2 reduction, with a corresponding yield of 18.8 μmol g -1 h -1 , 15 times higher than that of pure Bi 2 O 2 SO 4 , and CO selectivity reaching 97.1%. The results indicate that metal deposition enhances light absorption utilization efficiency and promotes the separation and transfer of photogenerated carriers. Additionally, the combination of in-situ FT-IR spectra and theoretical calculations reveal the molecular mechanisms of photocatalytic CO 2 reduction. This work discusses the synergistic effect of metal deposition and oxygen vacancies on photocatalytic reduction of CO 2 , providing a feasible method for constructing metal deposition structures with defects.
研究领域:
材料科学
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环境科学
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2024
·
IF 4.1
Qinghua Qu,Yuqiao Jiang,Linyan Cheng,Qingyuan Xue,Ranran Li,Cheng Fang,Hongping Li,Jing Ding,Hui Wan,Guofeng Guan
Covalent organic frameworks (COFs) with high specific surface area, ordered pore wall, modified porous surface and customizable chemical structure have been widely used in CO 2 capture. However, the screening of functionalized COFs suitable for CO 2 capture still relies on experiments, which will require a long experimental period with blindness and randomness. Herein, we chosed three electron withdrawing groups (–NO 2 , –CN and −Br) and three electron donating groups (–CH 2 NH 2 , –CH 3 , –OCH 3 ) to explore the effect of electron withdrawing ability of functional groups on the CO 2 adsorption capacity. Grand canonical Monte Carlo (GCMC) method was used to simulate the adsorption capacity of CO 2 over X-TpBD-COFs (X=–NO 2 , –CN, −Br, –CH 2 NH 2 , –CH 3 , –OCH 3 ). As the result, NO 2 -TpBD-COF had the highest adsorption capacity among the six functionalized X-TpBD-COFs at 100 kPa and 25 ℃ (49.37 cm 3 /g), while OCH 3 -TpBD-COF had the lowest adsorption capacity among them (23.51 cm 3 /g at 25 ℃ and 100 kPa). The order of binding energy was basically the same as the order of adsorption capacity when the synergistic interactions between functional groups and oxygen atoms in Tp were considered according to density functional theory (DFT). Molecular dynamics (MD) showed that the diffusion and distribution of CO 2 were mainly effected by pore structures. To verify the simulation results, NO 2 -TpBD-COF and OCH 3 -TpBD-COF were successfully prepared by solvothermal method. The CO 2 adsorption capacities of these two COFs were basically consistent with the conclusion obtained by the simulations. This study provided a way for simulation to guide accurate and rapid experimental design of COF materials for CO 2 capture.
研究领域:
材料科学
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环境科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Yan Xin,Binfei Li,Zhaomin Li,Zongyang Li,Bo Wang,Xiaopu Wang,Mengyuan Zhang,Weitao Li
During the CO 2 flooding process in fractured low-permeability oil reservoirs, the injected CO 2 is prone to channeling along fractures due to severe reservoir heterogeneity, resulting in poor development effect. The CO 2 -responsive gel system shows dual advantages in achieving CO 2 capture and plugging gas channeling to enhance oil recovery. This paper constructed a system with good CO 2 sensitivity based on long-chain alkyl amide propyl dimethyl tertiary amine first. Subsequently, the properties of the system before and after the response were evaluated through rheological test, and its microstructure was characterized by Cryo-TEM. The system exhibited good CO 2 responsiveness, transitioning from low-viscosity solution system to high-viscosity CO 2 -responsive gel system upon contact with CO 2 , with its viscosity increasing by nearly five orders of magnitude. The CO 2 -responsive gel demonstrated excellent shear resistance, viscoelasticity and shear self-repairing ability. The change of microstructure further verified the mechanism of molecules self-assembly in the system under the action of CO 2 . Then, a series of core physical simulation experiments were carried out to comprehensively evaluate the effects of different factors on the injection capacity, plugging characteristics, dynamic filtration damage performance and EOR effect of CO 2 -responsive gel. The gel maintained injectability while achieving an exceptional deep plugging effect, and the plugging rate reached 98.77%. It showed good characteristics of low filtration and permeability damage in low permeability reservoirs, effectively ensuring the fracture plugging effect. After the fracture was plugged by gel, the sweep range of CO 2 to the matrix significantly expanded, and the gas flooding recovery increased by 18.19–21.7%. Finally, the matrix-fracture dual-media chip model was used to conduct microfluidic experiment, the oil displacement characteristics in different displacement stages were visually clarified, and the synergistic plugging and oil displacement mechanism between the CO 2 -responsive gel and CO 2 was summarized. The research results can provide important insights for the green and efficient application of CO 2 -responsive gel in fractured low-permeability reservoirs.
研究领域:
石油工程
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化学工程
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）