SOLID STATE SCIENCES
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2025
·
IF 3.3
Feng-Jun Zhang,Zi-Chen Wang,Yu-Hong Niu,Jie Ma
For ultimate photocatalytic CO 2 reduction efficiency, In 2 O 3 synthesized via co-precipitation/calcination was architecturally integrated with Bi 2 MoO 6 through solvothermal assembly, constructing composite catalysts. In 2 O 3 incorporation triggered absorption edge red-shifting, quenched photoluminescence, and amplified photocurrent density. The 2 %-In 2 O 3 composite delivered 12.5 μmol/g/h CO yield under 300W xenon lamp – achieving a 2.5-fold enhancement versus pure In 2 O 3 and a 1.8-fold gain relative to pure Bi 2 MoO 6 . This superiority arose from heterostructuring induced by In 2 O 3 loading, which expedited photogenerated carrier mobility and elevated CO 2 conversion activity.
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高影响因子
Nature Communications
·
2025
·Vol. 16
·期 1
·1-9
·
IF 15.7
Wei Shilei,Hua Hang,Zhao Yuxuan,Luo Jingshan
Zero-gap membrane electrode assembly (MEA) CO 2 electrolysers offer high energy efficiency and promise for industrial application. However, the transport of carbonates within an anion exchange membrane (AEM) electrolyser leads to CO 2 loss, thereby limiting carbon utilization efficiency. Emerging acidic anolyte electrolysers using cation exchange membrane (CEM) can address this challenge but face critical stability issues, including accelerated hydrogen evolution reaction (HER) and persistent salt precipitation. Here, we propose a porous membrane (PM) as an alternative to the CEM in acidic anolyte electrolysers. The system demonstrates continuous operation at 100 mA cm −2 for 200 h without salt precipitation, while maintaining nearly 100% CO selectivity. Furthermore, large-scale device (100 cm 2 ) also shows stable performance. Mechanism analysis suggests that enhanced water permeation and bidirectional ion transfer are critical for achieving stable performance in acidic anolyte electrolysers. These findings offer a feasible approach for high-performance, stable and scalable acidic MEA CO 2 electrolysers.
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PubMed
高影响因子
RARE METALS
·
2025
·
IF 11
Wang Long-Yan,Fan De-Qi,Li Yi,Zhao Cheng-Xiao,Yang Xiao-Fei
Metalloporphyrins featuring structurally tunable aromatic macrocycles and versatile metal coordination sites are widely recognized as promising molecular catalysts for photocatalytic carbon dioxide reduction. However, their catalytic performances are constrained by rapid recombination of photogenerated charge carriers, insufficient charge transfer efficiency, and structural instability caused by molecular aggregation. Anchoring metalloporphyrins onto conductive substrates, in particular ultrathin two-dimensional (2D) nanostructures, can effectively accelerate interfacial charge transport efficiency, thereby improving photocatalytic activity toward CO 2 reduction. In this work, a novel 2D/2D heterojunction was designed and synthesized, which can serve as a highly efficient molecular catalyst for visible-light-driven CO 2 reduction. The abundant Co centers and N-sites in the assembled cobalt-coordinated porphyrin nanobelts can greatly enhance the adsorption and conversion of CO 2 . Meanwhile, the presence of few-layer Ti 3 C 2 MXene nanosheets enables the accelerated interfacial charge transport from photoexcited metalloporphyrin to Ti 3 C 2 MXene. Rapid electron transfer is verified by Kelvin probe force microscopy (KPFM), in situ attenuated total reflectance-Fourier transform infrared (ATR-FTIR), and irradiated X-ray photonelectron spectroscopy (XPS). As expected, compared to pristine porphyrin, the metalloporphyrin/Ti 3 C 2 MXene heterojunction shows a 12.5-fold increase in the photocatalytic activity for CO 2 reduction to CO. Graphical abstract
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2024
·
IF 3.8
Li Wang,Zhangmiao Ye,Caihong Lin,Yugao Wang,Jinping Li,Jiangfeng Yang
N2O/CO2 separation in the tail gas of adipic acid presents a significant challenge due to the closely resembling physical characteristics exhibited by CO2 and N2O. Herein, adsorption and separation performances of CO2 and N2O on FAU-type zeolite Y with different cations (Na+ and Ag+) were studied comprehensively. After Ag+ exchange, zeolite Y changes from a CO2-selective adsorbent to a N2O-selective adsorbent. AgY shows high N2O uptake (95.7 cm3/g) but relatively low adsorption heat (23.1 kJ/mol), making it suitable for N2O/CO2 separation. In situ Fourier transform infrared spectrometry indicates that N2O is successfully adsorbed on AgY. The breakthrough experiment reveals that AgY exhibits superior performance in the separation of N2O/CO2 at a flow rate of 20 mL/min while also exhibiting a favorable retention time and ratio of retention time with CO2 breakthrough time, which can reach up to 4.1 min and 0.24, respectively, which makes it an optimum N2O/CO2 separation material reported so far.
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CHEMICAL ENGINEERING SCIENCE
·
2025
·
IF 4.3
Lidong Wang,Chensheng Ma,Qin Dai,Kangkang Li,Kaiqi Jiang
Solvent degradation is the most critical challenge of amine-based CO 2 capture technology, which necessitates the development of chemically stable amine/amine blends to mitigate the absorbent degradation for industrial application. This study experimentally examined fourteen structurally different amines, namely the relatively stable cyclic, sterically hindered, and tertiary amines, to reveal the relationship between amine structure and chemical stability. The cyclic amines with a symmetrical ring structure greatly promote their oxidative stability, whilst the asymmetrical ring structure exhibited poor performance due to its relatively high C-N bond flexibility. The potential intramolecular interaction between the parent ring and the branched chain also reduced the stability of cyclic amines. While sterically hindered amines showed desirable oxidative stability thanks to the C-N bond protection by substitutions adjacent to amino group, their stability was very sensitive to the number of chain and the type of functional group surrounding to the amino group. Thermal stability of sterically hindered amines was also less satisfactory. It is observed that the amines with a rigid C-N bond, a longer branched chain connected to parent ring, and a preferable steric hinderance substantially promote the oxidative stability, with approximately 20 times less degradation compared to the benchmark MEA. Quantum calculation of bond dissociation energies (BDEs) of hydrogen-containing bonds were performed to reveal the atom position of radical formation that initiates the amine degradation. The potential degradation pathways were further predicted based on the positions of radical formation and the calculation of reaction Gibbs energy for possible degradation reactions. The analysis of heat stable salts products and the nitrogen distribution in the degraded solutions confirmed the bond cleavage position induced by radical formation and the reaction pathways, which clarified the potential amine oxidation mechanism. This work is anticipated to provide the generic principles to evaluate and develop the chemically stable amine solvent towards long-term operation of the amine process.
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CHEMICAL ENGINEERING SCIENCE
·
2024
·
IF 4.1
Wenlong Chen,Yuting Chen,Runwei Mo,Jiannong Wang
To reduce the amount of carbon dioxide (CO 2 ) already emitted into the atmosphere, various carbon capture, utilization, and storage (CCUS) technologies have been developed for climate and economic reasons in recent years. However, the state of art CCUS techniques suffer from deficiencies such as high cost, low yield, and harsh and discontinuous production conditions. In this work, we report a new thermal reduction method for continuously conversing CO 2 to methane (CH 4 ) by introducing sodium borohydride (NaBH 4 ) as a reductant under catalyst-free conditions. Experimental results show that CO 2 can be fully captured and converted to CH 4 and carbon monoxide (CO) and the selectivity efficiency of CO 2 to CH 4 can be achieved to be as high as 90% with the optimization of experimental conditions. Such a result originates from the high activity of NaBH 4 and high selectivity of the thermal reduction of CO 2 . To demonstrate one of the potential usages of the reduction products, we integrated the thermal reduction of CO 2 with the production of carbon nanotubes (CNTs). As long as CO 2 is supplied at the source end, the reduction products can undergo catalytic decomposition to produce a CNT fiber or film continuously at the final end. The present technique is featured with simple equipment setup, low cost, and continuous thermal reduction, thus providing a new pathway for the large-scale conversion of CO 2 into high-valued products for wide applications.
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高影响因子
JOURNAL OF ORGANIC CHEMISTRY
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2024
·
IF 3.3
Tianyu Zhu,Yue Xu,Zhenjiang Li,Jun He,Xin Yuan,Dong Qian,Tong Chang,Longlin Lu,Bo Chi,Kai Guo
A halide-free ionic pair organocatalyst was proposed for the cycloaddition of CO2 into epoxide reactions. Cholinium pyridinolate ionic pairs with three different substitution positions were designed. Under conditions of temperature of 120 °C, pressure of 1 MPa CO2, and catalyst loading of 5 mol %, the optimal catalyst cholinium 4-pyridinolate ([Ch]+[4-OP]−) was employed. After a reaction time of 12 h, styrene oxide was successfully converted into the corresponding cyclic carbonate, and its selectivity was improved to 90%. A series of terminal epoxides were converted into cyclic carbonates within 12 h, with yields ranging from 80 to 99%. The proposed mechanism was verified by 1H NMR and 13C NMR titrations. Cholinium cations act as a hydrogen bond donor to activate epoxides, and pyridinolate anions combine with carbon dioxide to form intermediate carbonate anions that attack epoxides as nucleophiles and lead to ring opening. In summary, a halide-free ionic pair organocatalyst was designed and the catalytic mechanism in the cycloaddition of CO2 into epoxides reactions was proposed.
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PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Zeyou Meng,Yuhao Hu,Xin Ye,Xiao Sun,Jun Hu,Zhen Wang,Jiabao Qiang,Sanping Chen,Gang Xie
To address the limitation of mono-pore mode SBA-15 on adsorption efficiency and the aggregation of amine groups within the confined pores, an innovative TEOS hydrolysis-driven dual-pore strategy to fabricate SBA-15-Dual-Mesopore (SBA-DMP) structure with covalent-grafted of 3-trimethoxysilylpropan-1-amine (APTMS) is proposed. Structural and thermodynamic characterizations reveal that this dual-mesopore design provides more CO 2 adsorption sites, and the larger mesopores exhibit a strong affinity for tetraethylenepentamine (TEPA) that significantly enhances its dispersion and incorporation efficiency. Of noted, for the first time, electron paramagnetic resonance (EPR) spectroscopy is employed to study the electronic interactions within amine-functionalized materials, indicating that APTMS-induced surface hydrogen bonds facilitate lone pair electron delocalization through electronic rearrangement, improving the local electronic density around secondary amines. Microcalorimetric studies, along with temperature-programmed desorption (TPD) and density functional theory (DFT) calculations, confirm that hydrogen bonding significantly enhances the reactivity of secondary amines, leading to a high CO 2 adsorption capacity of 5.83 mmol g −1 at 70 °C under 10 % CO 2 (60 % RH). The comprehensive evaluation of the SBA-DMP material demonstrates an excellent amine efficiency, adsorption stability, recyclability, and selectivity, highlighting its suitability for practical CO 2 capture. The dual-mesopore design with surface hydrogen bonding collectively advances CO 2 adsorption efficiency, offering a practical and effective solution for carbon capture.
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高影响因子
Journal of Energy Chemistry
·
2020
·
IF 7.216
Jin-Feng Liao,Ya-Ting Cai,Jun-Yan Li,Yong Jiang,Xu-Dong Wang,Hong-Yan Chen,Dai-Bin Kuang
The optoelectronic performance of CsPbBr 3 nanocrystal (NC) has been dramatically limited by the severe charge carrier recombination and its narrow light absorption range, which are anticipated to be resolved via coupling with plasmonic Au nanoparticle (NP). In view of this, CsPbBr 3 –Au nanocomposite is fabricated and further employed as a concept model to study the electronic interaction between perovskite NC and Au NP for the first time. It has been found that the excitation-wavelength dependent carrier transfer behavior exists in CsPbBr 3 –Au nanocomposite. Upon illumination with visible light ( λ >420 nm), photo-generated electrons in CsPbBr 3 can inject into Au with an electron injection rate and efficiency of 2.84 × 10 9 s −1 and 78%, respectively. The boosted charge separation is further translated into a 3.2-fold enhancement in CO 2 photocatalytic reduction activity compared with pristine CsPbBr 3 . On the other hand, when solely exciting Au NP with longer wavelength light ( λ >580 nm), the localized surface plasmon resonance (LSPR) induced hot electrons in Au NPs can transfer to CsPbBr 3 NC and further participate in photocatalytic reaction towards CO 2 reduction. The present study provides new insights into preparing plasmonic nanostructure to enhance the performance of perovskite based optoelectronic devices.
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高影响因子
JOURNAL OF MATERIALS SCIENCE
·
2018
·Vol. 53
·期 16
·11595-11606
·
IF 2.993
Wu Keliang,Dong Xuejun,Zhu Junfang,Wu Pengcheng,Liu Chang,Wang Yixi,Wu Jianning,Hou Juan,Liu Zhiyong,Guo Xuhong
The nanostructured heterojunction photocatalysts are considered promising in photocatalytic reduction in the carbon dioxide. Herein, we demonstrate a simple sol–gel and hydrolysis process to design nanostructured TiO 2 /ZnO heterojunction, by using the biological template celery stalk. The nanostructured photocatalyst consists of anatase TiO 2 and wurtzite ZnO nanoparticles. A well-connected heterojunction, with uniformly distributed nanoparticles, on the pores and folds of celery stems, is obtained. The enhanced specific surface area of 55.5 m 2 /g is achieved. The crystal structure, morphology and surface composition are investigated by electron microscopy, X-ray photoelectron spectroscopy and X-ray diffraction. Furthermore, we demonstrate the photocatalytic performance of as-synthesized nanostructure TiO 2 /ZnO heterojunction. The photocatalytic yield, of CO 2 reduction into CH 4 , exhibits a five times increase, from 0.55 to 2.56 µmol h −1 g −1 , for the nanocomposite as compared to the pure TiO 2 . This enhanced performance corresponds to the efficient charge transfer and hindrance in the recombination of electron–hole pairs due to the optimum band positions of ZnO and TiO 2 . This study demonstrates the potential of using biotemplates to design efficient photocatalysts to convert CO 2 into useful solar fuels.
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高影响因子
Frontiers of Chemical Science and Engineering
·
2020
·Vol. 15
·期 4
·882-891
·
IF 3.552
Fan Yiyi,Li Jinyong,Wang Saidi,Meng Xiuxia,Jin Yun,Yang Naitao,Meng Bo,Li Jiaquan,Liu Shaomin
Hydrogen fuel has been embraced as a potential long-term solution to the growing demand for clean energy. A membrane-assisted separation is promising in producing high-purity H 2 . Molecular sieving membranes (MSMs) are endowed with high gas selectivity and permeability because their well-defined micropores can facilitate molecular exclusion, diffusion, and adsorption. In this work, MXene nanosheets intercalated with Ni 2+ were assembled to form an MSM supported on Al 2 O 3 hollow fiber via a vacuum-assisted filtration and drying process. The prepared membranes showed excellent H 2 /CO 2 mixture separation performance at room temperature. Separation factor reached 615 with a hydrogen permeance of 8.35 × 10 −8 mol·m −2 ·s −1 ·Pa −1 . Compared with the original Ti 3 C 2 T x /Al 2 O 3 hollow fiber membranes, the permeation of hydrogen through the Ni 2+ -Ti 3 C 2 T x /Al 2 O 3 membrane was considerably increased, stemming from the strong interaction between the negatively charged MXene nanosheets and Ni 2+ . The interlayer spacing of MSMs was tuned by Ni 2+ . During 200-hour testing, the resultant membrane maintained an excellent gas separation without any substantial performance decline. Our results indicate that the Ni 2+ tailored Ti 3 C 2 T x /Al 2 O 3 hollow fiber membranes can inspire promising industrial applications.
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高影响因子
ACS Sustainable Chemistry & Engineering
·
2020
·
IF 7.632
Shuhui Wang,Jiawei Zhan,Kui Chen,Asad Ali,Linghui Zeng,He Zhao,Wanglai Hu,Lixin Zhu,Xiaoliang Xu
The visible-light-driven CO2 reduction efficiency is largely restrained by the negative photoabsorption and high recombination rate of electron–hole pairs. It is an effective method to increase the efficiency of CO2 photoreduction by doping alkali metal elements to engineer the electronic properties of the catalyst. Here, we report a new study on the potassium-doped g-C3N4 (K-CN) being used for CO2 reduction irradiated by visible light. DFT calculations and XPS tests show that the potassium doping is interlayer doping, changing the electronic structure of g-C3N4. The higher ID/IG value indicates more structural distortion and defects caused by K doping. K-CNs have enhanced visible-light absorption, and PL spectra demonstrate that the introduction of potassium advances the separation and transmission of photoexcited charge carriers, further confirmed by transient photocurrent response experiment. Under visible light, K-CN-7 achieved efficient CO2 reduction without any noble metal as a cocatalyst, with CO formation rates of 8.7 μmol g–1 h–1, which is 25 times that of ordinary g-C3N4. Our work further validates the importance of inhibiting e–/h+ recombination in improving solar energy conversion efficiency while also bringing hope for efficient solar fuel production using g-C3N4.
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