Molecular Catalysis
·
2025
·
IF 4.9
Jun Ma,Shiyan Li,Bing Xu,Wei Chu,Qian Jiang,Yuefeng Liu
Converting CO 2 from the coal chemical industry into natural gas via methanation reaction, coupled with green hydrogen, is a promising strategy for reducing carbon emissions. While Ni-based catalysts are cost-effective and widely used for CO 2 methanation, their performance is often hindered by low temperatures activity. We confined LaO x species within the mesoporous silica (mSiO 2 ) channels to serve as a support for Ni-based CO 2 methanation catalysts. The results demonstrate that LaO x introduction (3.9 wt%) significantly improves CO 2 conversion from 38.2 % to 74.4 %, while enhancing CH 4 selectivity from 94.8 % to 99.7 % at 300 °C. Interestingly, excessive La loading does not noticeably reduce the promotion efficiency. Detailed characterization revealed that ultrafine LaO x species anchored within silica framework improved the dispersion and reduction of Ni nanoparticles and served as strong basic sites to promote CO 2 dissociation. In-situ DRIFT and isotope studies demonstrated that LaO x facilitated the hydrogenation of formate intermediates, enhancing both CO 2 conversion and CH 4 selectivity. In addition, LaO x endowed the support with hydrogen spillover capability, enabling active H from Ni nanoparticles to migrate to LaO x sites and accelerate the conversion of formate intermediates into CH 4 . These results underscore the potential of LaO x -modified mesoporous silica to optimize Ni-based catalysts, offering valuable guidance for the design of high-performance CO 2 hydrogenation catalyst supports.
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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
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2025
·
IF 6
Qinghai Long,Jing Wang,Tiantian Ping,Shufeng Shen
Nonaqueous absorbents have shown great potential in lowering regeneration energy for energy-efficient CO 2 capture. The effect of reaction media with varying solvent characteristics (polarity, solubility parameter and dielectric constant) on kinetic behaviors deserves to be discovered. In this work, CO 2 absorption flux against CO 2 partial pressure was determined in a stirred cell reactor at temperatures of 283.2–303.2 K with 1.0–5.0 mol L −1 2-(butylamino)ethanol (BAE) in nonaqueous 2-butoxyethanol (2-BE). Physicochemical properties and the physical mass transfer coefficients were also measured and represented by proposed correlations. The overall reaction rate constants were derived under the well-defined pseudo-first-order regime conditions. The partial reaction order with respect to BAE was found to be about 2.0 in 2-BE and 1.0–1.3 in water respectively, which reveals that the formation of ionic products may be highly depressed in solvent with low Hansen solubility parameter (HSP) resulting in the increasing reaction order. The overall third-order kinetic data can be well represented by termolecular mechanism model with AARD of 10.5 %. The findings will provide fundamental support for further pilot-scale performance demonstration.
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CATALYSIS LETTERS
·
2025
·Vol. 155
·期 10
·1-11
·
IF 2.4
Zhou Jie,Yu Wen-Wang,Meng Xiang-Guang,Li Wen,Chu Dan-Dan
The development of catalytic systems capable of in situ capturing carbon dioxide (CO 2 ) from flue gas under ambient pressure and subsequently converting it into high-value chemicals holds significant practical importance for reducing atmospheric CO 2 levels and advancing the chemical industry. In this study, deep eutectic solvents (DESs) composed of an imidazolium salt and 3-aminobenzyl alcohol were synthesized and employed to catalyze the cycloaddition of CO 2 from simulated flue gas (15% CO 2 + 85% N 2 ) with epoxides. This catalytic system exhibited excellent catalytic activity, the yield of cyclic carbonate reached up to 94.3% upon reacting under simulated flue gas conditions at 55 °C and 1 atm for 24 h. The effects of temperature, reaction time and catalyst dosage on catalytic efficiency were investigated. The scope of various epoxides was also explored. Furthermore, the catalytic system is readily recyclable, maintaining nearly consistent catalytic activity over five cycles. The catalytic mechanism was clarified via FT-IR and NMR spectroscopic analyses, and a plausible cycloaddition reaction pathway was proposed. Graphical
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Catalysts
·
2025
·Vol. 15
·期 9
·889
·
IF 4
Lijun Xue,Yuxuan Wang,Chenhui Qiu,Hui Wan
Developing highly efficient photocatalysts for CO2reduction remains a great challenge. The large band gap and poor charge carrier dynamics are the major factors limiting the performance of Bi4Ti3O12(BTO). Herein, a series of La-doped Bi4Ti3O12(BLaxTO) nanosheets were synthesized and further modified by NaBH4hydrogenation to create surface defect-rich H-BLaXTO nanosheets. Characterizations and theoretical calculations confirmed that the synergistic effect of La doping and hydrogenation significantly enhanced visible-light absorption, promoted charge separation, and improved the electron reduction capacity. When applied to photocatalytic CO2reduction, the H-BLa0.2TO catalyst achieved a superior CH3OH production rate of 7.90 μmol·g−1·h−1, which is 5.6 times higher than that of pristine Bi4Ti3O12. Moreover, the H-BLa0.2TO catalyst maintained excellent stability over four consecutive cycles. This study offers an integrated strategy for constructing high-performance bismuth-based photocatalysts through elemental doping and defect engineering.
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Energy & Environmental Science
·
2022
·Vol. 15
·期 8
·3494-3502
·
IF 39.714
Lianpeng Song,Zhong Liang,Mingzi Sun,Bolong Huang,Yaping Du
The selectivity in the electrocatalysis of carbon dioxide reduction reaction (CO2RR) has attracted tremendous attention but still faces a great challenge. Constructing an interface has become an advanced strategy to effectively modulate electroactivity and selectivity. Herein, we report the synthesis of a CeO2/Bi3NbO7 fibrous tubular structure through a simple electrospinning method, which has shown a much-improved selectivity of 84.73% towards formic acid with remarkable durability in the CO2RR. Theoretical calculations have demonstrated that the construction interface has supplied highly electroactive regions with efficient electron transfer, which not only improves the adsorption of key adsorbates but also alleviates the reaction energy barriers. The modulation induced by the interface enables the high selectivity and yield of HCOOH. This work has supplied a novel and advanced strategy to utilize the interfacial effect in developing superior CO2RR electrocatalysts in the future.
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ADVANCED FUNCTIONAL MATERIALS
·
2025
·
IF 19
Li Yin,Meiling Li,Hailun Xia,Shanshan Mao,Fangyuan Gai,Hao Wang
The gas separation performance of hybrid carbon molecular sieve membranes is critically influenced by the particle size of the fillers. Herein, ZIF-8 crystals of different sizes (≈50 nm, ≈500 nm, and ≈1 µm) are used as fillers to synthesize a series of ZIF-8-derived-carbon hybrid carbon molecular sieve membranes with high filler loading. As the ZIF-8 crystal size increases from nanoscale to microscale, the CO 2 permeability of the resulting hybrid carbon molecular sieve membrane for a CO 2 /CH 4 binary mixture increases, reaching 9965 Barrer with a selectivity of 28.05. This trend highlights a clear correlation between filler size and gas separation performance of the hybrid carbon molecular sieve membranes. Microscale ZIF-8-derived-carbon offers synergistic advantages by providing abundant hierarchical pores for molecular sieving and continuous, long pathways for efficient gas transport, while preventing particle aggregation under high loading. Our finding provides valuable insights for the further development of high-performance hybrid carbon molecular sieve membranes.
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Journal of Cleaner Production
·
2023
·
IF 11.1
Jie Qi,Yang Ge,Qingping Li,Xin Lv,Xiaojiang Li,Na Wang,Hongsheng Lu
Paraffin wax has caused obvious detrimental consequences to the extraction for fossil fuels, and posed environmental challenge due to the absence of cleaner methods for paraffin wax removal. A cleaner and sustainable approach for paraffin wax removal was developed using the switchable polarity solvents (SPS). Three SPS with low polarity, including dipropylamine (DPA), ethylbutylamine (EBA), and dibutylamine (DNBA) were selected for paraffin wax removal. Compared with bubbling CO 2 into SPS straightway, the transformation of the polarity quantified by normalized polarity energy confirms the addition of water is benefit to enlarge the polarity scope. Paraffin wax is removed at the initial state and separated at the final state by CO 2 -induced polarity transformation of SPS. The dissolution rates for paraffin wax of DPA and EBA reached 0.071 g/min and 0.062 g/min, which surpassed that of traditional solvents, such as o-xylene (0.045 g/min) and Petroleum ether (0.017 g/min), indicating that these selected SPS is suitable for paraffin wax removal. The paraffin wax dissolution behaviors of SPS can be accurately matched using modified Apelblat models with root-mean-square deviation of 1.085%. With the addition of water, more than 99% of paraffin wax is separated from DPA and EBA by introducing CO 2 within 10mins, which is a better alternative method for energy-intensive distillation process . The introduction of water is indispensable for improving the separation efficiency, since it enlarged the polarity difference between solvents and paraffin wax. The thermal behavior of separated paraffin wax detected by Differential Scanning Calorimetry remained steady, and there were negligible residual solvents detected indicate the feasible separation of paraffin wax. Both SPS and water are recovered upon N 2 /80 °C, which retain good recyclability for paraffin wax removal. These findings confirms the applicability of SPS in the sustainable and cleaner removal of paraffin wax. The use of SPS provides an alternative and promising approach for paraffin wax removal for ensuring the demands of low-energy consumption and environment.
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CHINESE JOURNAL OF POLYMER SCIENCE
·
2017
·Vol. 36
·期 1
·18-24
·
IF 1.692
Jing Xian-Wu,Huang Zhi-Yu,Lu Hong-Sheng,Wang Bao-Gang
A series of triblock copolymers, containing a CO 2 -switchable block poly(2-(dimethylamino)ethyl methacrylate) (PDM) block and two symmetrical hydrophilic blocks polyacrylamide (PAM), were synthesized using atom transfer radical polymerization (ATRP) method. The pH and conductivity tests showed that the triblock copolymer exhibited switchable responsiveness to CO 2 , i.e. a relatively low conductivity of solution could be switched on and off by bubbling and removing of CO 2 , and the triblock copolymer aqueous solution displayed a CO 2 -switchable viscosity variation. The changes were all attributed to protonation of tertiary amine groups in PDM blocks and proven by 1 H-NMR. Cryogenic transmission electron microscopy and dynamic light scattering characterization demonstrated that the viscosity variation was the result of a unilamellar vesicle-network aggregate structure transition. The release of rhodamine B from the vesicles with and without CO 2 stimuli showed the potential application in drug delivery domains; after CO 2 bubbling, the drug release rate could be accelerated. Finally, reasonable mechanism of CO 2 -switchable morphology changes and CO 2 -induced drug release was proposed.
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CHEMICAL ENGINEERING SCIENCE
·
2026
·
IF 5.1
Xiang Duan,Qingpeng Cheng,Xiaotong Sun,Shaohui Xiong,Wei Liu,Maofeng Ding,Jiayan Yan,Qicheng Zhang,Ye Tian,Prasert Reubroycharoen,Jorge Gascon,Xingang Li
Heterophase junction engineering enables intrinsic promotion without additives. • Electron-rich S v obtained via 1T → 2H charge transfer boosts intrinsic activity. • Heterophase junctions redistribute network with formate pathway promoted. Thermocatalytic hydrogenation of CO 2 to methanol offers a promising route for carbon recycling and renewable energy storage, yet achieving high activity and methanol selectivity under low-temperature conditions remains challenging. Herein, we construct MoS 2 catalysts with tunable 1T/2H phase ratios by phase engineering, enabling the formation of well-defined heterophase junctions. Through interfacial charge transfer, metallic 1T domains serve as intrinsic electron donors to sulfur vacancies on adjacent 2H domains, thereby modulating their electronic structure. This heterophase-junction-mediated electronic regulation enhances the intrinsic catalytic activity while steering methanol synthesis toward the formate-mediated pathway. Consequently, the optimized 1T/2H-700 catalyst containing 4.7% 1T phase exhibits approximately 1.6-fold intrinsic activity compared with the pure 2H phase catalyst, achieving an impressive 6.3% CO 2 conversion and 87.1% methanol selectivity at the low temperature of 200 °C. More importantly, this work establishes heterophase junction engineering as an intrinsic-promoter strategy for electronic regulation of catalytic sites, providing a new catalyst design principle beyond conventional promoter-assisted systems. Download: Download high-res image (138KB) Download: Download full-size image
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Journal of Materials Chemistry A
·
2018
·Vol. 6
·期 42
·21110-21119
·
IF 9.931
Qiaoqiao Mu,Wei Zhu,Gangbin Yan,Yuebin Lian,Yuanzhou Yao,Qin Li,Yuyu Tian,Peng Zhang,Zhao Deng,Yang Peng
The development of efficient and economical catalysts for photocatalytic reduction of CO2 into chemical feedstocks is highly desirable for addressing both the global energy crisis and carbon emission problem. Herein, a series of carbonized cobalt composites derived from bimetallic Zn/Co zeolitic imidazolate frameworks (C-BMZIFs) are synthesized and used as the co-catalysts for [Ru(bpy)3]2+ mediated photocatalytic CO2 reduction under visible light irradiation. Varying the Zn/Co ratio allows regulation of the size of Co active sites, which further differentiates their catalytic activity towards CO2 reduction and H2 evolution, resulting in tunable CO/H2 ratio in the produced syngas. Among all investigated configurations, the C-BMZIF with a Zn/Co ratio of 3 : 1 demonstrates the highest CO yield of 1.1 × 104 μmol g−1 h−1, owing to the optimal balance between the quantity of active sites and the activity of each individual site. Consequently, this work provides insight into the design of stable MOF-derived co-catalysts for efficient photo-reduction of CO2, and offers an alternative solution for photocatalytic syngas production with tunable CO/H2 ratio.
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CATALYSIS TODAY
·
2019
·
IF 4.888
Yunxia Zhao,Hui Ge,Yuanyuan Miao,Jiaxin Chen,Wei Cai
Metal-organic framework (MOF) materials have significant advantages for capturing CO 2 . To further improve the CO 2 adsorption performance of MOFs, a compound material of l -arginine modified graphene oxide (GO) with MOFs (MOF/GO-Arg) was synthesized. Introduction of amino acid-functionalized lamellar GO into MOF material not only generated new pores at their interface to improve the adsorption of the MOF but also promoted the CO 2 capture at low humidity. The structural and chemical properties of the parent components and composite materials were analyzed by X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR), N 2 adsorption-desorption, thermal analysis and scanning electron microscopy (SEM). The dynamic CO 2 adsorption properties of the materials were compared under different temperatures, flow rates and humidities. Three kinetic models were used to fit the adsorption curves of the as-synthesized adsorbents under different conditions, and then the optimal dynamic model was determined. Since the reusability of the adsorbents is especially important for the use of these materials in practice, the CO 2 adsorption was repeated for 10 cycles under optimal temperature, flow rate and high humidity conditions.
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CHINESE JOURNAL OF CATALYSIS
·
2023
·
IF 16.5
Zhuogen Li,Qadeer Ul Hassan,Weibin Zhang,Lujun Zhu,Jianzhi Gao,Xianjin Shi,Yu Huang,Peng Liu,Gangqiang Zhu
The H 2 evolution is generally considered a competing reaction in photocatalytic CO 2 reduction reaction (CO 2 RR) using H 2 O as the proton source. However, the reducing gas H 2 generated from H 2 O splitting can be the proton source in CO 2 RR under the enhanced dynamic role of the thermal effect. The reverse water gas shift (RWGS) reaction, a CO 2 hydrogenation reaction, should occur in photothermal environment owing to thermodynamically and kinetically favorable. Herein, nanostructured metal-semiconductor contact consisting of Pt nanoparticles (NPs) supported on SrTiO 3– δ nanosheets with rich oxygen vacancies (Pt-OVs-STO) was constructed for investigating its feasibility and efficiency in the RWGS reaction under photothermal effect. Our experimental results substantiate that the H 2 generated by H 2 O splitting effectively contributes to the RWGS reaction over Pt-OVs-STO system. The Pt 0 NPs not only efficiently facilitate surface charge transfer, but also lower the energy barrier of the O–H bond breaking, H 2 releasing, and RWGS reaction, thereby showing an outstanding CO 2 RR performance. The strong interaction between the Pt 0 NPs and SrTiO 3– δ has been extensively demonstrated by a series of experimental characterizations and density functional theory calculations. This work elucidates the relation between H 2 evolution and RWGS reaction over Pt 0 /SrTiO 3– δ structure in photothermal catalytic CO 2 RR using H 2 O as the proton source and provides new perspectives for subsequent CO 2 RR.
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