Molecular Catalysis
·
2025
·
IF 4.9
Lu Ren,Bin Wang,Yueli Wen,Maohong Fan,Zhaoxiong Huang,Wenxuan Li,Wei Huang,Jing Li,Jianping Guo
Acid-base synergistic effect is crucial in adjusting the catalytic performance of CO 2 hydrogenation to methanol, an efficient CO 2 emission reduction and carbon recycle strategy. Two MOFs-derived catalysts (CZ-MIL, CA-ZIF) with opposite acid-base properties were tailored by using MIL-68 (Al) and ZIF-8 (Zn) as precursors, and the above two MOFs precursors were hybridized (C-ZAx) to control the acid-base property of the catalyst. C-ZA0.6 (molar ratio of MIL-68 (Al) to ZIF-8 (Zn)=0.6) exhibits a promising catalytic performance with CO 2 conversion of 8.9 %, methanol selectivity of 61.85 %, and STY of 117.02 mg mL −1 ·h −1 at 4 MPa and 523 K. Combined with comprehensive analysis, it is found that methanol selectivity is closely related to weak acid sites arising from the residual skeleton of MIL-68. Acid-base synergy facilitates the hydrogenation of CO 2 to methanol. The basic sites are responsible for adsorbing and activating CO 2 , and the acidic site helps to stabilize CO* and facilitate the further hydrogenation to methanol. This work provides a new idea and feasible method for enhancing the catalytic performance of CO 2 hydrogenation to methanol.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2025
·
IF 6.3
Xiting Tao,Chunyan Zhang,Zhiming Yang,Chao Yao,Xiazhang Li
The conversion of carbon dioxide and water into fuels through artificial photosynthesis is of great significance for achieving carbon neutrality. However, this reaction faces great challenge due to the sluggish kinetics. Herein, high-entropy spinel (NiFeMnCoCu) 3 O 4 nanoparticles supported on palygorskite (Pal) were synthesized using a facile sol-gel method, and the composite was employed for photocatalytic CO 2 reduction coupled with biomass-derived 5-hydroxymethylfurfural (HMF) oxidation. The hydrochloric acid-modified Pal (H-Pal) facilitated the generation of high concentrations of oxygen vacancies in (NiFeMnCoCu) 3 O 4 , inducing a localized surface plasmon resonance (LSPR) effect, expanding the light absorption range to the near-infrared region and releasing high-energy hot electrons, thereby enhancing the photocatalyst's photothermal conversion capability. The HMF oxidation along with dehydrogenation addressed the issue of slow kinetics while harnessing the potential of biomass resources. Moreover, the high concentration of oxygen vacancies significantly improved the separation efficiency of charge carriers, favoring the enhanced photocatalytic CO 2 reduction and HMF oxidation ability of the (NiFeMnCoCu) 3 O 4 /H-Pal composite. Current study provides a novel strategy for the conversion of CO 2 and the high-value utilization of biomass.
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Small
·
2025
·
IF 12.1
Teng Zhang,Xueya Dai,Yihong Yu,Xin Cui,Yunlong Li,Gaowu Qin,Wei Qi,Song Li
Electrochemical conversion of CO 2 into value-added multi-carbon products is highly attractive for CO 2 utilization using sustainable electricity energy. However, achieving high ethanol selectivity of copper-based catalysts remains challenging due to the competing side reactions such as ethylene formation. Herein, a novel electrocatalyst, PANI-Ag/Cu-OH is reported, comprising of polyaniline-supported silver single atoms coupled with hydroxyl-modified copper clusters. Tandem reduction of CO 2 into ethanol with a high selectivity is realized by coupling CO formation on Ag site and further reduction on hydroxylated Cu sites. The synergistic approach enables a high Faradaic efficiency of 68.9% for ethanol with a current density of −263.8 mA cm −2 at −0.78 V versus RHE in alkaline media. CO-TPD and in situ infrared spectra studies reveal that strong CO adsorption and Cu + species stabilized by hydroxyl groups are crucial for asymmetric C–C coupling and stabilization of the ethanol intermediates, leading to the enhanced ethanol selectivity.
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JOURNAL OF CATALYSIS
·
2025
·
IF 6.5
Mingming Chu,Wenjing Sun,Songbing Yu,Yuanhang Li,Fangyu Zhu,Lijuan Yu,Yongyong Cao,Xuebo Cao,Yiming Li
Covalent organic frameworks (COFs) that incorporate heterocycles featuring multiple nitrogen atoms, such as triazine, bipyridine, and heptazine, are seen as promising heterogeneous photocatalysts for CO 2 photoreduction, while the substantial effect of N-atom relative locations in this transformation has rarely been systematically studied. Herein, a collection of isostructural porphyrin-based COF catalysts bearing bipheyl, 2–2′-bipyridine and 3–3′-bipyridine are judiciously designed for CO 2 photoreduction under simulated sunlight irradiation (1000 W/m 2 ). As results, comparing with the frequently used biphenyl and 2–2′-bipyridine unit, the porphyrin COF incorporating 3–3′-bipyridine yields a significant enhancement in photoelectric properties, and the CO production rate of 3–3′-Bpy-COF is 2 and 10 times higher than that of 2–2′-Bpy-COF and Bp-COF. Insights on the origin of the improved photocatalytic activity and reaction mechanism are further investigated, revealing above tiny variation of N sites results in a larger dipole moment for the 3–3′-Bpy-COF, facilitating the separation and transfer of photogenerated excitons. Moreover, The X-ray Photoelectron Spectroscopy (XPS) and Density Functional Theory (DFT) calculations reveal that the 3–3′-bipyridine N-atoms can strategically adjust the electron density surrounding the M−N4 active center of porphyrins, which stabilize the *COOH intermediate and reduce the energy barrier of the rate-determining step. This work highlights the collaborative influence of porphyrin and the steric location of N atoms within COFs photocatalysts for CO 2 reduction reaction, offering a new insight to design COFs endowed with exceptional capabilities for photocatalysis.
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Korean Journal of Materials Research
·
2025
·Vol. 35
·期 8
·352-365
·
IF 0.3
Haixia Wang,Yilei Sun,Yao Liu,Kunjie Li,Zeda Meng,Won-Chun Oh
The catalyst materials 0N-Cu-MOF, 1N-Cu-MOF, and 2N-Cu-MOF were successfully synthesized usinga solvothermal method, and using different concentrations of nitrogen-modified Cu organic frameworks (xN-Cu-MOF). Characterizations using X-ray diffraction (XRD), scanning electron microscopy (SEM), fourier transform infrared (FT-IR) spectroscopy, X-ray photoelectron spectroscopy (XPS), and Brunauer-Emmett-Teller (BET) surface area analysis showed that 1N-Cu-MOF had the largest SSA and pore size among the three materials synthesized. 1N-Cu-MOF exhibited the largest pore size and specific surface area among the three materials, which had a decisive effect on CO2 reduction. In addition, stability and CO2 reduction reaction (CO2RR) activity were evaluated by linear sweep voltmeter, cyclic voltmeter, electrochemical impedance spectroscopy, and time flow tests. Faradaic efficiency (FE) was determined by product analysis. Among the three catalyst materials, 1N-Cu-MOF showed the best catalytic performance at 50 mA·cm-2 (maximum current density). The charge transfer resistance was 8.23 Ω, the average current density was 19.9 mA·cm-2, and the FE of methane (CH4) production showed a high efficiency of 70.45 % when tested for 12 h at an overpotential of -0.35 V (to-RHE).
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AICHE JOURNAL
·
2025
·
IF 4
Qiangbing Shi,Kaige Jia,Xiangping Zhang,Chuan Wang,Paul Cobden,Anna-Maria Beregi Amnéus,David Muren,Xiaoyan Ji
The development of advanced absorbents for effectively capturing carbon dioxide is crucial in mitigating greenhouse gas emissions. This study introduced a series of deep eutectic solvents (DESs) for CO 2 capture and identified the most promising DESs with the stepwise screening method based on their absorption capacity, absorption rate, thermal stability, desorption efficiency, and apparent activation energy. Consequently, compared to the monoethanolamine (MEA), in the 30 wt% aqueous solutions, [1,2,3-Triazolium chloride][diethylenetriamine] ([TrizCl][DETA]) and [Piperazinium chloride][diethylenetriamine] ([PzCl][DETA]) improved the CO 2 absorption capacities by 31% and 34%, absorption rates by 12% and 30%, and the amounts of CO 2 desorbed by 42% and 23%, as well as reduced the apparent activation energies by 9% and 28%, respectively. Meanwhile, their thermal stabilities (degradation onset temperatures, T onset ) were enhanced by 101% and 32%, respectively. The FTIR and NMR analyses were conducted to provide deeper insights into the chemical absorption mechanism of CO 2 by the DESs.
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JOURNAL OF MEMBRANE SCIENCE
·
2025
·
IF 9
Qian-Qian Li,Yang Li,Heng Mao,Yan-Mei Zhang,Qiu-Ying Zhang,Xin-Ru Chen,Zi-Cong Shan,Xian-Zhe Zhou,Li-Hao Xu,Zhi-Ping Zhao
Mixed matrix membranes (MMMs) have emerged as a critical platform for molecular separation, especially carbon capture from point-emission sources. In this study, a series of novel MMMs were fabricated by incorporating the bimetallic Ag/Zn-ZIF-8 nanoparticles into the poly (ether-block-amide) (Pebax) matrix for efficient CO 2 /N 2 separation. The SEM, EDS, XRD, FTIR, XPS, TGA, N 2 adsorption-desorption measurements were employed to elucidate the microstructures and physicochemical properties of the resultant nanoparticles and membranes. The bimetallic coordination-induced optimization modulated the inherent structure of ZIF-8 framework and enhanced CO 2 affinity, thereby forming the CO 2 -selective transport channels over N 2 . The incorporation of Ag + promoted the uniform dispersion of Ag/Zn-ZIF-8 nanoparticles in Pebax matrix, indicating the excellent polymer-filler interfacial compatibility. Impressively, the resulting membrane achieved the superior separation performance with a CO 2 permeability of 359 Barrer and a CO 2 /N 2 selectivity of 53, which were 2.5 and 1.4 times higher than that of the pristine Pebax membrane. Besides, the introduction of Ag/Zn-ZIF-8 nanoparticles enhanced the thermal and mechanical stability of the membrane, ensuring the potential for long-term operation. These findings herein advance the rational design and preparation of high-performance MMMs for sustainable carbon capture.
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Journal of Environmental Chemical Engineering
·
2025
·Vol. 14
·期 1
·120850
·
IF 7.2
Xiaohua Tong,Enyang Zhang,Guangran Shao,Ming Yuan,Boyi Song,Wangqing Zhang
Polymer blending is a simple and cost-effective method to improve the gas separation performance of polyimide membranes, thereby potentially overcoming the inherent permeability/selectivity trade-off effect. However, its application still faces challenges, since only a few polymers are miscible with polyimides, and the mechanical property of the membranes usually reduces significantly after polymer blending. Herein, we prepare membranes by blending polyimide containing bulky isopropyl substituents with a small amount of polar polymers such as polyacrylonitrile (PAN). The resultant blend membranes using PAN as additive not only possess excellent gas separation performance but also maintain good mechanical property. For example, when 0.8 wt% PAN is added, the corresponding blend membrane displays a high CO 2 permeability of 632.2 Barrer and a high CO 2 /CH 4 selectivity of 23.4 under humidified condition, close to the 2008 Robeson upper bound, which is attributed to the formation of micro-phase separation structure within the blend membranes. Moreover, the tensile strength of the blend membranes using 0.8 wt% PAN as additive is only 12 % lower than that of the pure polyimide membrane. In addition, the blend membranes using PAN as additive show remarkable stability against physical aging and outstanding long-term operation stability, suggesting their great prospect for natural gas purification and biogas upgrading.
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Nanomaterials
·
2025
·Vol. 16
·期 1
·35
·
IF 4.3
Wenjing Wu,Zichao Yang,Min Zhang,Zhongjie Guan,Jianjun Yang
Photocatalytic reduction of carbon dioxide is a very effective strategy to address the energy crisis and greenhouse effect. TiO2is a widely used semiconductor photocatalyst, which has excellent catalytic activity, excellent chemical stability and low toxicity. Nevertheless, TiO2still has some inherent limitations, such as: wide band gap, high carrier recombination rate, and low adsorption activation ability for carbon dioxide. These drawbacks severely restrict its further application in the photocatalytic reduction of CO2. In this study, cotton-like blue C/TiO2NTs are successfully synthesized through the in situ growth of TiO2nanotubes on the MIL-125(Ti)-derived C/TiO2precursor. The experimental results revealed that the CO production rate of the cotton-like blue C/TiO2NTs was 1.84 times that of C/TiO2and 3.78 times that of TiO2nanotubes. These results clearly demonstrate that the cotton-like blue C/TiO2NTs exhibit a broad spectral response, a large specific surface area, and an abundance of oxygen vacancies. This research provides new insights into the design of titanium dioxide-based photocatalytic materials and opens up a promising avenue for enhancing the performance of titanium dioxide in the photocatalytic reduction of carbon dioxide.
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ENERGY & FUELS
·
2025
·
IF 5.3
Qiulin Ye,Dongdong Wang,Jiabao Lv,Minghui Tang,Angjian Wu,Yaqi Peng,Shengyong Lu
The electrocatalytic CO2 conversion offers a sustainable pathway for generating ecofriendly chemicals and fuels while simultaneously enabling the storage of intermittent renewable energy. Herein, CuPd bimetallic catalysts were specifically designed through displacement reaction, with a magnetron sputtering Cu film as a substrate. The optimized CuPd catalyst achieved an ethylene Faradaic efficiency (FE) of 51.07% and a C2+ FE of 82.18% at a 200 mA/cm2 current density. In situ Raman spectroscopy indicates that the CuPd electrode exhibited a high local surface pH during the CO2 reduction reaction, which was favorable for C–C coupling. The observation of the *OCCOH intermediate by in situ FTIR, combined with density functional theory calculations, confirms that the CuPd surface promotes C–C coupling instead of direct hydrogenation. This mechanistic insight explains why the addition of Pd enhances the selectivity for C2+ products.
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Small
·
2025
·
IF 12.1
Deguang Ji,Zi Yang,Yaxiong Yao,Yichao Hou,Zidong He,Pengfei Da,Wei Shen,Li An,Yuanmiao Sun,Pinxian Xi,Chun-Hua Yan
Copper-based catalysts show considerable promise in the electrochemical CO 2 reduction reaction (CO 2 RR) for the production of hydrocarbons and oxygenates, particularly methane (CH 4 ), which is a highly reduced product. The high-valent state of copper (Cu) exerts a positive influence on the formation pathway of CH 4 , but the reduction potential will lead to a decrease in the valence state during CO 2 RR. In this study, a highly crystalline and structurally well-defined Y 2 Cu 2 O 5 catalyst is constructed to stabilize Cu 2+ with the orderly alternating Y─O skeleton layer, owing to the strong bonding interaction. The Y 2 Cu 2 O 5 exhibits a remarkable enhancement in CH 4 selectivity compared to CuO (up to 9.59-folds), achieving a selectivity of 61.3% at 300 mA cm −2 and 58.4% at 400 mA cm −2 , together with good stability. In situ attenuated total reflectance Fourier transform infrared spectra (ATR-FTIR) and density functional theory (DFT) calculations reveal that the presence of the Y─O skeleton layer in Y 2 Cu 2 O 5 significantly enhances the adsorption of *CO intermediate, and accelerates its hydrogenation process, facilitating the conversion of CO 2 to CH 4 . This work highlights Y─O skeleton-mediated stabilization of Cu 2+ for efficient electroreduction of CO 2 to CH 4 , providing valuable insights into the design of efficient electrocatalysts for CO 2 conversion.
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ACS Applied Polymer Materials
·
2025
·
IF 4.7
Jun Cai,Yang Song,Yunfei Yu,Jie Chen,Chao Wang,Xiaoli Ding,Xue Yang,Jianqiang Meng
Ion gel membranes exhibit high efficiency and environmental friendliness for CO2/N2 separation, but their poor mechanical strength and inability to self-heal after physical damage hinder their industrial application. To overcome these limitations, we propose an efficient one-pot method for preparing dual-network (DN) ion gel membranes with enhanced gas separation and self-healing properties. This method involves constructing dual self-healing networks: the first network (FN), formed through a Schiff base reaction between O,O’-bis(2-aminopropyl)poly(propylene glycol)-block-poly(ethylene glycol)-block-poly(propylene glycol) (H2N–PPG-PEG-PPG-NH2) and 1,3,5-benzenetricarboxaldehyde (BTC), and the second network (SN), consisting of polyurethane (PU) featuring a quadruple hydrogen-bonded cross-linked network. By optimizing the ratio of the two networks to 5:2 and adjusting the ionic liquid content ([EMIM]TFSI) to 60 wt %, the resulting DN membrane demonstrates exceptional CO2 gas separation performance, with a CO2 permeability (PCO2) of 726 Barrer and a selectivity (αCO2/N2) of 23. This underscores the potential of this process for effective gas separation applications. Furthermore, compared to conventional ion gel membranes, the DN membranes exhibit significant improvements in mechanical properties and self-healing capabilities, while maintaining high CO2 permeability and selectivity.
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