INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2025
·
IF 3.9
Bowen Tan,Danru Xu,Mengmeng Jin,Bolun Yang,Zhun Hu,Jingjun Liu
Cerium dioxide (CeO2) with different morphologies was synthesized via a hydrothermal method and applied to the carbonylation of glycerol with CO2. Subsequent characterization through H2-TPR and catalytic activity tests demonstrated that CeO2 nanorods exhibited the highest oxygen storage/release capacity as well as enhanced catalytic performance compared to other morphologies. CeO2 nanorods were thus further modified through hydrogen reduction at varying temperatures, aiming to tune the density of the oxygen vacancies. Characterization via BET, NH3-TPD, CO2-TPD, XPS, and ESR indicated that variations in morphology and reduction temperature influenced the microstructural characteristics and the strength of the acid–base sites of the catalysts. Notably, hydrogen reduction created more oxygen vacancies in the CeO2 nanorods, with the concentration of these vacancies increasing with higher reduction temperatures. Furthermore, the catalytic activity of CeO2 in glycerol carbonylation with CO2 showed a positive correlation with the concentration of oxygen vacancies. Optimizing CeO2 catalysts can enhance its performance in activating CO2, providing new ideas for industrial CO2 resource utilization and carbon capture technology development.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
·
IF 9.4
San-Mei Wang,Shenghua Zhou,Shu-Guo Han,Dong-Dong Ma,Wenbo Wei,Qi-Long Zhu
Constructing local microenvironments is one of the important strategies to improve the electrocatalytic performances, such as in electrochemical CO 2 reduction (ECR). However, effectively customizing these microenvironments remains a significant challenge. Herein, utilizing carbon nanotube (CNT) heterostructured semi-open Co-N 2 O 2 catalytic configurations (Co-salophen), we have demonstrated the role of the local microenvironment on promoting ECR through regulating the location of hydroxyl groups. Concretely, compared with the maximum Faradaic efficiency (FE) of 62% for carbon monoxide (CO) presented by Co-salophen/CNT without a hydroxyl microenvironment, the designed Co-salophen-OH 3 /CNT, featuring hydroxyl groups at the Co-N 2 O 2 structural opening, shows remarkable CO 2 -to-CO electroreduction activity across a wide potential window, with the FE of CO up to 95%. In particular, through the deuterium kinetic isotope experiments and theoretical calculations, we decoded that the hydroxyl groups act as a proton relay station, promoting the efficient transfer of protons to the Co-N 2 O 2 active sites. The finding demonstrates a promising molecular design strategy for enhancing electrocatalysis.
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Surfaces and Interfaces
·
2025
·
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.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Meidan Que,Peihong Ma,Yabo Wang,Yanbo Sun,Xiangwei Bai,Lili Gao,Jin Chen,Jian Wei,Hui Li
NH 2 -MIL-125 with abundant porosity and specific interactions with CO 2 molecules, has been demonstrate great potential in the field of photocatalytic CO 2 reduction. However, conventional NH 2 -MIL-125 and their composites much lower CO 2 photoreduction efficiency in aerobic environments because of the O 2 competition. To circumvent the issue, this study modifies NH 2 -MIL-125 through crystal facet engineering to enhance its selective CO 2 adsorption and photocatalytic efficiency in the environment of impurity CO 2 . The results indicate that NH 2 -MIL-125 featuring (101) crystal planes can sustain elevated catalytic activity in low-concentration CO 2 environments. In a pure CO 2 atmosphere, NM-5 achieves a CO production rate of 159.66 μmol·g −1 after 4 h, 1.85 times greater than the unmodified NH 2 -MIL-125. Under conditions simulating flue gas (5 % CO 2 ) and ultra-low CO 2 concentrations (0.15 % CO 2 ), NM-5 maintains CO production rates of 3.18 μmol·g −1 and 0.95 μmol·g −1 , respectively, representing 1.63 and 1.73 times the production rates of NM. Furthermore, theoretical calculations indicate that CO 2 exhibits a higher adsorption energy (−1.34 eV) compared to N 2 and O 2 (−0.67 eV and −0.15 eV) on the (101) crystal plane, which reveals the preferential adsorption of CO 2 on the (101) crystal planes. This study involves a novel strategy for optimizing MOFs crystal planes and provides significant insights into achieving efficient photocatalytic CO 2 reduction under aerobic conditions.
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Nature Communications
·
2025
·Vol. 16
·期 1
·1-10
·
IF 15.7
Song Zhilong,Fan Linfeng,Lu Shuaihua,Ling Chongyi,Zhou Qionghua,Wang Jinlan
Directly generating material structures with optimal properties is a long-standing goal in material design. Traditional generative models often struggle to efficiently explore the global chemical space, limiting their utility to localized space. Here, we present a framework named Material Generation with Efficient Global Chemical Space Search (MAGECS) that addresses this challenge by integrating the bird swarm algorithm and supervised graph neural networks, enabling effective navigation of generative models in the immense chemical space towards materials with target properties. Applied to the design of alloy electrocatalysts for CO 2 reduction (CO 2 RR), MAGECS generates over 250,000 structures, achieving a 2.5-fold increase in high-activity structures (35%) compared to random generation. Five predicted alloys— CuAl, AlPd, Sn 2 Pd 5 , Sn 9 Pd 7 , and CuAlSe 2 are synthesized and characterized, with two showing around 90% Faraday efficiency for CO 2 RR. This work highlights the potential of MAGECS to revolutionize functional material development, paving the way for fully automated, artificial intelligence-driven material design.
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JOURNAL OF RARE EARTHS
·
2025
·
IF 7.2
Lihua Hu,Suning Zhang,Peishen Zhao,Jie Yang,Gongde Wu,Wei Xu
The catalytic direct synthesis of dimethyl carbonate (DMC) from CO 2 and methanol is a crucial approach to utilizing CO 2 and producing high-value chemicals. However, the high stability of the CO 2 molecule imposes thermodynamic limitations on this reaction pathway, along with challenges related to insufficient catalyst activity and stability. Currently, solutions primarily focus on developing efficient catalyst. Herein, La-doped CeO 2 nanoflower catalysts (La x CeO 2 ) were synthesized via hydrothermal method. Characterization reveals that La doping optimizes the pore structure and enriched oxygen vacancies, thereby enhancing catalytic performance. Notably, La 0.1 CeO 2 exhibits the largest pore size and highest oxygen vacancy content, achieving a remarkable DMC productivity of 9.42 mmol/g under 140 °C, 4 MPa of CO 2 , and 3 h of reaction, surpassing pure CeO 2 nanoflowers. Based on experimental findings and in-situ diffuse infrared Fourier transform analysis, a plausible reaction pathway was proposed. This work underscores the potential of La x CeO 2 nanoflowers as efficient catalysts for sustainable CO 2 conversion to DMC.
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ACS Catalysis
·
2024
·
IF 11.3
Bin Chen,Dehuan Shi,Renxia Deng,Xin Xu,Wenxia Liu,Yang Wei,Zheyuan Liu,Shenghong Zhong,Jianfeng Huang,Yan Yu
Revealing the synergistic catalytic mechanism involving multiple active centers is crucial for understanding multiphase catalysis. However, the complex structures of catalysts and interfacial environments pose a challenge in thoroughly exploring the experimental evidence. This study reports the utilization of a CuNi dual-atom catalyst (Cu/Ni–NC) for the electrochemical reduction of CO2. It demonstrates a high Faradaic efficiency of CO exceeding 99%, remarkable reaction activity with a partial current density surpassing –300 mA cm–2, and prolonged stability for more than 5 days at a current density of –200 mA·cm–2. Operando characterization techniques and density functional theory calculations reveal that Ni atoms function as active sites for the activation and hydrogenation of CO2, while Cu atoms serve as active sites for the dissociation of H2O, supplying protons for the subsequent hydrogenation process. Moreover, the electronic interactions between Ni and Cu atoms facilitate the formation of *COOH and the dissociation of H2O, illustrating a synergistic reduction of CO2 at the dual-atom sites.
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ACS Omega
·
2024
·
IF 3.7
Qing Guo,Ze Li,Xuanxiang Zeng,Dan Li,Huiming An,Li Zhao,Liang Tao,Qiang Li
Reduction of the reservoir permeability during supercritical CO2 fracturing caused significant reservoir damage, which directly affects the crude oil recovery rate. This investigation explored a novel thickener for supercritical CO2 fracturing fluid, this CO2 thickener not only effectively improves the viscosity and rheological properties of CO2 fracturing fluid but also contributes to reduce reservoir damage and improve permeability. The research results indicated that the synthesized CO2 thickener (3 wt %) can increase the apparent viscosity of supercritical CO2 fracturing fluid to 7 mPa·s, and a 9% matrix permeability damage rate and a 0.5 mD permeability decrease value are shown in a 3% CO2 fracturing fluid. However, 3 wt % of commercial CO2 thickener only increases the apparent viscosity of supercritical CO2 fracturing fluid to 3 mPa·s, while the reservoir damage rate increases to 13%. Two thickeners exhibit completely different damage capabilities to the reservoir, and the synthesized CO2 thickener shows excellent characteristics of reducing reservoir permeability and is also conducive to protecting shale reservoirs. Furthermore, supercritical CO2 fracturing fluid containing synthetic thickeners has better temperature and shear resistance compared with commercial thickeners. This may be because the synthesized thickener and the micro grid formed by supercritical CO2 reduce the adsorption in shale crevices, but a large amount of commercial thickeners can adsorb on the surface of shale.
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ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Lingjia Ma,Jiongliang Yuan,Zhaotao Liu,Yiqing Luo,Yuning Su,Kunye Zhu,Zefeng Feng,Huihua Niu,Shuaishuai Xiao,Jianjun Wei,Xu Xiang
The electrocatalytic synthesis of high-value-added urea by activating N2 and CO2 is a green synthesis technology that has achieved carbon neutrality. However, the chemical adsorption and C–N coupling ability of N2 and CO2 on the surface of the catalyst are generally poor, greatly limiting the improvement of electrocatalytic activity and selectivity in electrocatalytic urea synthesis. Herein, novel hierarchical mesoporous CeO2/Co3O4 heterostructures are fabricated, and at an ultralow applied voltage of −0.2 V, the urea yield rate reaches 5.81 mmol g–1 h–1, with a corresponding Faraday efficiency of 30.05%. The hierarchical mesoporous material effectively reduces the mass transfer resistance of reactants and intermediates, making it easier for them to access active centers. The emerging space-charge regions at the heterointerface generate local electrophilic and nucleophilic regions, facilitating CO2 targeted adsorption in the electrophilic region and activation to produce *CO intermediates and N2 targeted adsorption in the nucleophilic region and activation to generate *N ═ N* intermediates. Then, the electrons in the σ orbitals of *N ═ N* intermediates can be easily accepted by the empty eg orbitals of Co3+ in CeO2/Co3O4, which presents a low-spin state (LS: t2g6eg0). Subsequently, *CO couples with *N ═ N* to produce the key intermediate *NCON*. Interestingly, it was discovered through in situ Raman spectroscopy that the CeO2/Co3O4 catalyst has a reversible spinel structure before and after the electrocatalytic reaction, which is due to the surface reconstruction of the catalyst during the electrocatalytic reaction process, producing amorphous active cobalt oxides, which is beneficial for improving electrocatalytic activity.
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Catalysis Science & Technology
·
2024
·Vol. 14
·期 14
·4019-4028
·
IF 4.4
Yang Yang,Liqiang Zhang,Jiaben Wang,Hao Song,Xiao Zhang,Xiang Gao
Indium oxide is widely used in the photothermal catalytic reduction of CO2. However, the high bandgap and relative low CO2 adsorption capacity limit its application. Herein, we report a simple and cost-effective strategy to modify In2O3 with hydrogen treatment and Cu doping to form a Cu–In2O3−x catalyst with a lower bandgap and enhanced CO2 adsorption properties. The catalyst can absorb more visible light and effectively reduce the activation energy of the intermediate in the CO2 reduction route, thus demonstrating superior performance in the photothermal catalytic reduction of CO2. Moreover, the Cu–In2O3−x catalyst can maintain almost 100% product selectivity over a wide range of reaction conditions and reaches the highest yield compared to other doping noble metals (Ru, Pt, and Rh). This catalyst synthesis strategy provides practical application prospects for CO green manufacturing, as well as inspiration for the performance improvement of other catalytic materials.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2025
·
IF 3.9
Wei Zheng,Haiyan Jiang,Chaoran Wang,Shaojuan Zeng,Xiaochun Zhang,Haifeng Dong,Lu Bai,Xiangping Zhang
Carbon dioxide (CO2) separation plays a vital role in environmental protection and resource reuse. A potential approach to achieving satisfactory CO2 separation is combining the benefits of ionic liquids (ILs) and membranes. In this work, the IL-LDH nanosheets were obtained by functionalized IL modifying layered double hydroxides (LDH) and used to construct the Pebax/IL-LDH mixed matrix membranes (MMMs). The X-ray diffraction (XRD), Fourier transform infrared (FTIR) spectroscopy, and X-ray photoelectron spectroscopy (XPS) spectra analysis displayed that the IL was successfully grafted to the LDH nanosheets. The characterizations of MMMs showed that the introduction of IL-LDH reduces the crystallinity of the Pebax membrane, and there are hydrogen bond interactions between fillers and Pebax. The IL modification strengthens the membranes with better CO2 affinity and improves the interfacial compatibility between Pebax and LDH. Meanwhile, the CO2-philic nanochannels formed by the slits of IL-LDH nanosheets facilitate CO2 transport in MMMs. Such inherent properties of the IL and LDH conjunctly contribute to the improvement of the CO2 separation performance of membranes. The optimum Pebax/IL(20)-LDH MMM has a high CO2 permeability of ∼388 barrer at 30 °C, which is approximately 2.9 times that of pure Pebax, and the CO2/CH4 selectivity does not change significantly. Besides, the Pebax/IL(20)-LDH MMM exhibited a notable increase in CO2 permeability as the working temperature increased, ultimately attaining ∼576 barrer at 50 °C.
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NEW JOURNAL OF CHEMISTRY
·
2025
·
IF 2.5
Yafei Sang,Xiaolong Jia,Pengpeng Wu,Xiangquan Yan,Xiaotao Kuang,Quan Feng,Jiahao Qiao,Min Chen,Jian Zhang,Xiuli Yan,Tao Chang
The porous organic polymers HIP-Br-1 and HIP-Br-2 rich in bromine anions were prepared by quaternization one-pot method. The contents of N and Br in HIP-Br-1 reached 15.93 wt% and 6.94 wt% respectively. These high content of bromine ions combined with rich mesoporous and macroporous structures gave the materials good catalytic ability. The material has moderate adsorption heat (28-36 kJ/mol). The catalytic experiment shows that HIP-Br-1 has good catalytic performance. Under the mild conditions of 0.4 MPa CO2, 60 oC, and 9 h, without any cocatalyst and solvent, 93% of propylene oxide can be converted to cyclic carbonate. The catalyst has good repeatability, and the conversion efficiency to cyclic carbonate did not significantly decrease after four catalytic experiments. Density functional theory (DFT) shows that HIP-Br-1 can effectively activate PO and CO2, thereby enhancing the catalytic activity of cycloaddition reactions. This work explores the one-step synthesis of ion-type porous organic polymers rich in nitrogen atoms.
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