JOURNAL OF MOLECULAR STRUCTURE
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2025
·
IF 4.7
Si-Mian Liu,Qian Liang,Mu-Lan Yao,Xiao Wang,Long Tang,Er-Lin Yue,Ji-Jiang Wang,Xiang-Yang Hou
The excessive existence of CO 2 in the atmosphere has caused serious environmental problems. Therefore, how to capture, selectively adsorb, and the effective utilization of CO 2 into useful chemicals has attracted widespread attention. In particular, the exploration of combining CO 2 capture with conversion has rarely been reported. Herein, two isometric metal-organic frameworks (MOFs) Cd 3 (ntba) 2 -(2,2′-bipy) 2 ] n (MOF1), and Co 3 (ntba) 2 (2,2′-bipy) 2 ] n (MOF2) were successfully obtained. Under normal temperature and pressure conditions, based on the ideal specific surface area porosity, MOF1 and MOF2 exhibit super adsorption and separation ability for CO 2 . The maximum adsorption capacity and separation ratio are 54.3 cm 3 g -1 (MOF1), 64.2 cm 3 g -1 (MOF2), and 16.9 (MOF1, CO 2 /CH 4 ), 192.7 (MOF1, CO 2 /N 2 ), 117.8 (MOF1, CO 2 /O 2 ), 22.6 (MOF2, CO 2 /CH 4 ), 130.3 (MOF2, CO 2 /N 2 ), 59.1 (MOF2, CO 2 /O 2 ), respectively. Under optimal reaction conditions, the MOF1 and MOF2 as catalysts demonstrate outstanding efficiency and reaction selectivity in catalyzing cycloaddition conversion reaction of CO 2 , achieving yields of 96% and 93%, respectively. The catalytic reaction produced useful chemical products via a novel method integrating CO 2 capture and conversion, eliminating the economic costs associated with CO₂ purification and enabling the economical utilization of CO₂ . Thus, this work presents a novel strategy for the CO 2 utilization in mixed gases and can also provide valuable references for related research.
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FUEL
·
2025
·
IF 7.5
Langlang Qin,Yunfei Gao,Caiyun Han,Qiannan Ding,Shuang Wang,Jinping Li
Photothermal hydrogenation of CO 2 to methanol using renewable H 2 represents a promising strategy for mitigating the greenhouse effect and the energy crisis. MoS 2 has been investigated as an effective catalyst for CO 2 hydrogenation in thermal catalysis. However, till now, the photothermal catalysis of MoS 2 for enhanced methanol synthesis has been rarely reported. In this study, we synthesized and investigated MoS 2 with a series of morphological changes from nanoflower, nanosheet to bulk structures. Characterization revealed that the nanosheet MoS 2 possesses the highest specific surface area and the most abundant active Sv sites. Performance tests indicated that under standalone thermal catalysis, the turnover frequency (TOF) for methanol synthesis follows the order: nanosheet > nano-flower > bulk for MoS 2 . However, the light-enhancement effects under photothermal catalysis exhibited a different trend with respect to morphological structure. It was discovered that bulk MoS 2 , which possesses the least specific surface area and Sv, showed the best light-enhancement effect with 102.45 % increase in methanol yield. It is hypothesized that the light-enhancement effect is more related to more exposed planar sites, which do not align linearly with specific surface area and Sv. These are evidenced by physiochemical characterizations, photoelectric response experiments and performance tests. These findings could offer important insights into future catalyst design for MoS 2 -type materials with both enhanced thermocatalytic activity and light-enhancement effect.
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Nanomaterials
·
2025
·Vol. 15
·期 24
·1903
·
IF 4.3
Reshalaiti Hailili,Yiming Gan
The development of versatile photocatalysts is crucial for comprehensive solutions to the intertwined challenges of the energy crisis and environmental pollution. This study presents a novel Bi3TiNbO9/Bi2MoO6(BTNO/BMO) heterojunction fabricated via a solvothermal method. Advanced characterization techniques verified the successful synthesis of the as-integrated BTNO/BMO heterostructure. The BTNO/BMO composite exhibited superior performance in multiple applications: efficient degradation of tetracycline reaching 90.2%, removal of gaseous nitric oxide (NO), and photocatalytic reduction of carbon dioxide (CO2) to carbon monoxide (CO) with a yield of 51.3 μmol·g−1. The constructed Type-II heterojunction demonstrated a remarkable ability to suppress charge recombination, thereby significantly enhancing the photocatalytic activity. This work highlights the dual-functional capability of the BTNO/BMO heterojunction for simultaneous environmental purification and fuel production, providing a promising material platform and a strategic design concept for sustainable technological development.
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PubMed
高影响因子
Nanomaterials
·
2025
·Vol. 15
·期 23
·1777
·
IF 4.3
Haihong Zhao,Lei Li,Jiaxin Li,Feiqi Yan,Wenhao Wang,Mingxia Zhao
In this work, a novel mixed-component bimetallic metal–organic framework (MOF) composite material was synthesized via a solvothermal approach, and its structural and textural properties were systematically characterized using X-ray diffraction (XRD), scanning electron microscopy (SEM), N2adsorption/desorption analysis, and transmission electron microscopy (TEM). Furthermore, the single-component adsorption isotherms of CO2and N2were experimentally measured and fitted to the Langmuir–Freundlich model. The CO2/N2selectivity of the composite was evaluated based on the ideal adsorption solution theory (IAST). The results demonstrated that the addition of Zn2+significantly enhanced the specific surface area and improved the CO2adsorption capacity (3.97 mmol/g at 35 °C and 1 bar), with an increase of 31.5% in comparison with the Cu-BTC/MCFs (3.02 mmol/g). Meanwhile, the Zn-Cu-BTC/MCFs had good recyclability and CO2/N2selectivity up to 12.5 determined via IAST (CO2:N2= 85:15).
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CHEMISTRY OF MATERIALS
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2025
·
IF 7
Jiangquan Lv,Yin Gao,Hanyang Liu,Zimin Han,Guoqing Feng,Rui Yang
Renewable-powered electrochemical CO2 reduction (ECO2R) provides a sustainable route to convert CO2 into valuable fuels and chemicals. However, conventional ECO2R systems face high energy costs due to the sluggish oxygen evolution reaction (OER) at the anode. Replacing the OER with biomass electrooxidation (e.g., glycerol oxidation reaction, GOR) can lower energy consumption while coproducing high-value chemicals. However, the construction of an efficient and cost-effective bifunctional catalyst remains a challenge. Herein, we design a low-cost, bifunctional Ni12P5@NCNT catalyst with a bamboo-like nanotube morphology for coupled ECO2R and GOR. The Ni12P5@NCNT exhibits exceptional performance, achieving 82% CO selectivity at −0.7 V vs RHE in ECO2R and a 95% Faradaic efficiency for formate production in GOR. The integrated system significantly reduces overpotential (219 mV) compared to conventional ECO2R //OER setups. Experiments reveal that the strong electronic interaction between Ni12P5 and NCNT enhances the CO2/glycerol adsorption and accelerates charge transfer, boosting both ECO2R and GOR activity. This work provides a promising strategy for co-upgrading CO2 and glycerol into valuable products using nonprecious metal catalysts.
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CHEMISTRY-A EUROPEAN JOURNAL
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2025
·
IF 3.7
Jianjian Yi,Tiaolong Lv,Guoxiang Zhang,Xu Wang,Xianglin Zhu,Yubo Zhou,Li Li,Xingwang Zhu,Xiaozhi Wang
Amorphous/crystalline catalysts can effectively integrate the advantages of both phases, overcoming the low active site density in crystalline phases and the poor charge separation in amorphous ones. In this work, we report an alkali salt-assisted partial phase transition strategy to synthesize amorphous/crystalline CoMnO x -400 nanosheets for photocatalytic CO 2 reduction. As a result, the as-prepared CoMnO x -400 demonstrates superior CO production performance (146.09 µmol g −1 h −1 , 93.6% selectivity), significantly outperforming amorphous CoMnO x -260 (66.65 µmol g −1 h −1 ) and crystalline CoMnO x -500 (89.52 µmol g −1 h −1 ). Supported by systematic characterizations, we propose that the high efficiency of CoMnO x -400 is attributed to two factors: (i) the charge migration between amorphous and crystalline phases across the seamless contact interface can enhance charge separation efficiency, and (ii) the amorphous domains can provide abundant surface defective active sites for CO 2 adsorption and activation. This work highlights the critical role of phase engineering, particularly the construction of amorphous/crystalline structures, in advancing solar-driven catalytic applications. Graphical This work presents an alkali salt-assisted annealing method to precisely synthesize CoMnO x with tunable crystallinity and systematically elucidating the structure-activity dependency between crystallinity and CO 2 photoreduction performance.
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CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Senshen Yu,Pengfei Lv,Pan Xue,Kai Wang,Qian Yang,Junhui Zhou,Meng Wang,Ling Wang,Biqiang Chen,Tianwei Tan
Natural photosynthesis plays an important role in maintaining environmental carbon balance. Taking inspiration from this, we developed a light-driven, enzymatic nanosystem for the highly selective production of formic acid from CO 2 . The system combines photocatalytic graphitic carbon nitride (g-C 3 N 4 ) with two natural enzyme catalysts, carbonic anhydrase (CA) and formate dehydrogenase (FateDH), encapsulated in ZIF-8, a porous metal-organic framework (MOF). Efficient in situ regeneration of reduced nicotinamide adenine dinucleotide (NADH) is realized through visible-light irradiation of g-C 3 N 4 with a suitable redox potential (−0.3 V (NHE)). The introduction of ZIF-8 ensures a large amount of loaded protein with little damage to enzyme activity, and its encapsulation of CA and FateDH shortens the distance between the enzymes. This is conducive to increasing the diffusion of substances during the CO 2 -to-formic acid cascade reaction, thus improving the reaction efficiency. This work is expected to provide new insight into the design and development of highly selective, artificial photosynthesis systems to efficiently convert CO 2 into fuels, chemicals, and other materials.
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Small
·
2023
·Vol. 20
·期 7
·2306576
·
IF 13.3
Wenbo Liu,Ning Wang,Yongjun Wu,Qianyi Zhang,Xiaoyan Chen,Yanmei Li,Rui Xu
The widespread acceptance of nonaqueous rechargeable metal–gas batteries, known for their remarkably high theoretical energy density, faces obstacles such as poor reversibility and low energy efficiency under high charge–discharge current densities. To tackle these challenges, a novel catalytic cathode architecture for Mg–CO 2 batteries, fabricated using a one-pot electrospinning method followed by heat treatment, is presented. The resulting structure features well-dispersed molybdenum carbide nanodots embedded within interconnected carbon nanofibers, forming a 3D macroporous conducting network. This cathode design enhances the volumetric efficiency, enabling effective discharge product deposition, while also improving electrical properties and boosting catalytic activity. This enhancement results in high discharge capacities and excellent rate capabilities, while simultaneously minimizing voltage hysteresis and maximizing energy efficiency. The battery exhibits a stable cycle life of over 250 h at a current density of 200 mA g −1 with a low initial charge–discharge voltage gap of 0.72 V. Even at incredibly high current densities, reaching 1600 mA g −1 , the battery maintains exceptional performance. These findings highlight the crucial role of cathode architecture design in enhancing the performance of Mg–CO 2 batteries and hold promise for improving other metal–gas batteries that involve deposition–decomposition reactions.
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ChemSusChem
·
2024
·Vol. 18
·期 7
·e202401046
·
IF 7.5
Habib Ullah,Zakir Ullah,Zafar A. K. Khattak,Muhammad Tahir,Eunji Kang,Francis Verpoort,Hyun You Kim
Graphical Herein, we report a solvothermal synthesis of a hydrazone-linked covalent organic framework (COF) towards solvent-free cycloaddition reaction of CO 2 and epoxides at ambient pressure. This functionalized cobalt-doped COF works well for various aromatic substrates with electron-withdrawing or donating groups and internal epoxides with a high yield of >99 % and 100 % selectivity. Covalent organic frameworks (COFs) constitute an evolving class of permanently porous and ordered materials, and they have recently attracted increased interest due to their intriguing morphological features and numerous applications in gas storage, adsorption, and catalysis. However, their low aqueous stabilities and tedious syntheses generally hamper their use in heterogeneous catalysis. Nonetheless, a capable and water-stable heterogeneous catalytic system for coupling CO 2 /epoxides to generate industrially important cyclic carbonates is still of great interest. Herein, exceedingly water- and thermally stable 2D-cobalt-impregnated hydrazone-linked fibrous COFs are reported as a catalyst for CO 2 /epoxide coupling reactions at ambient pressure. The functionalized cobalt (Co)-doped COFs demonstrated excellent catalytic activities with the high TONs (80925) and TOFs (6466 h −1 ), outperforming reported heterogeneous catalysts for CO 2 /epoxide coupling at ambient pressure. We found that the Co 2+ ions within the COF matrix catalyze CO 2 cycloaddition through density functional theory calculations. We also confirmed the excellent structural stability and consistent activity of Co-doped COFs up to ten repeating cycles.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2020
·
IF 3.573
Yang Wang,Sidi Wang,Zhen Li,Liwei Sun,Xiaoyu Yang,Shaokun Tang
UiO-66 nanocrystals were synthesized by supercritical reaction crystallization with anhydrous zirconium chloride as the metal precursor, terephthalic acid as the ligand, and a small amount of N,N-dimethylformamide (DMF) and formic acid as cosolvents in supercritical CO2. In our work, the product UiO-66 obtained exhibits typical octahedral morphology with a specific surface area of 1092 m2/g and concentrated micropore diameters of 0.77, 1.05, and 1.73 nm. The thermal decomposition temperature of the product is 450 °C. It was found that the adsorption selectivity of UiO-66 for Congo red is much higher than those for methylene blue and methyl orange, which can reach up to over 1300 mg/g. The adsorption process conforms to the second-order adsorption kinetics curve, and the adsorption isotherm fits into the Langmuir model. Meanwhile, the adsorbent UiO-66 possesses good cycle stability and its adsorption performance remains excellent after seven cycles.
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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
·
2019
·
IF 4.978
Yunwu Yu,Junhai Wang,Yan Wang,Wenhao Pan,Changwei Liu,Peng Liu,Lianjie Liang,Changwei Xu,Yunxue Liu
Phenolphthalein-based cardo poly(ether ether ketone) (PEEKWC)/polyethyleneimine (PEI) crosslinking membranes were prepared by solution casting followed by solution reaction at room temperature. The effects of reaction time and PEI content on the membrane structure and gas separation performances were investigated. Light transmittance measure and AFM evidenced the relationship between the microphase separation in PEEKWC-PEI membranes and reaction time. The CO 2 permeability increased with the PEI content, while the N 2 and CH 4 permeability remained nearly constant. This result indicated that only CO 2 was transported by the solution–diffusion mechanism and also that PEI exhibited a positive contribution as a fixed carrier for CO 2 facilitated transport. Meanwhile the PEEKWC-PEI crosslinking membranes showed higher selectivities than the pure PEEKWC membrane. The highest CO 2 /N 2 and CO 2 /CH 4 selectivities were about 131 and 122 increasing from 33 and 30, respectively. The crosslinking structure of membranes improved the CO 2 permeability stability.
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ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Wen-Gang Cui,Yan-Ting Li,Lei Yu,Hongbo Zhang,Tong-Liang Hu
Selective hydrogenation of CO2 to methanol is a “two birds, one stone” technology to mitigate the greenhouse effect and solve the energy demand–supply deficit. Cu-based catalysts can effectively catalyze this reaction but suffer from low catalytic stability caused by the sintering of Cu species. Here, we report a series of zeolite-fixed catalysts Cu/ZnOx(Y)@Na-ZSM-5 (Y is the mass ratios of Cu/Zn in the catalysts) with core–shell structures to overcome this issue and strengthen the transformation. Fascinatingly, in this work, we first employed bimetallic metal–organic framework, CuZn-HKUST-1, nanoparticles (NPs) as a sacrificial agent to introduce ultrasmall Cu/ZnOx NPs (∼2 nm) into the crystalline particles of the Na-ZSM-5 zeolite via a hydrothermal synthesis method. The catalytic results showed that the optimized zeolite-encapsulated Cu/ZnOx(1.38)@Na-ZSM-5 catalyst exhibited the space time yield of methanol (STYMeOH) of 44.88 gMeOH·gCu–1·h–1, much more efficient than the supported Cu/ZnOx/Na-ZSM-5 catalyst (13.32 gMeOH·gCu–1·h–1) and industrial Cu/ZnO/Al2O3 catalyst (8.46 gMeOH·gCu–1·h–1) under identical conditions. Multiple studies demonstrated that the confinement in the zeolite formwork affords an intimate surrounding for the active phase to create synergies and avoid the separation of Cu–ZnOx interfaces, which results in an improved performance. More importantly, in the long-term test, the Cu/ZnOx(1.38)@Na-ZSM-5 catalyst exhibited constant STYMeOH with superior durability benefitted from its fixed structure. The current findings demonstrate the importance of confinement effects in designing highly efficient and stable methanol synthesis catalysts.
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