Small
·
2024
·Vol. 20
·期 34
·2401914
·
IF 13
Zhaohui Fang,Xiaoyang Yue,Quanjun Xiang
Metal halide perovskite quantum dots (QDs) are widely studied in the field of photocatalytic CO 2 due to their strong light absorption and long carrier migration length. However, it can not exhibit high catalytic performance because of the radiative recombination and the lack of effective catalytic sites. Metal organic frameworks (MOFs) encapsulated QDs can not only solve the aforementioned problems, but also maintain their own unique characteristics with ultra-high specific surfaces area and abundant metal sites. In this work, lead-free bismuth-based halide perovskite QDs are encapsulated into Zr-based MOF (UiO-66), which combines the advantages with high power conversion efficiency of QDs and the high surface area and porosity of UiO-66. In addition, benefiting from the close contact between the Cs 3 Bi 2 Br 9 QDs and the UiO-66 enables the photogenerated electrons in the QDs to be rapidly transferred to the MOF. As a result, the Cs 3 Bi 2 Br 9 @UiO-66 composite exhibits a higher yield for photocatalytic CO 2 reduction than that of the prepared large-sized composite of Cs 3 Bi 2 Br 9 and UiO-66.
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Journal of Materials Chemistry A
·
2024
·
IF 10.7
Xi Chen,Wei Zhou,Xu Fang,Cheng Li,Die Cong,Tie Yu,Wei-Qiao Deng,Chengcheng Liu
Photocatalytic CO2 reduction to syngas has recently garnered substantial interest due to its mild reaction conditions, high safety, and environmental sustainability. However, the efficiency of syngas production remains relatively low. In this study, we have developed metallosalen-based poly(ionic liquid)s (PILs) to enhance syngas production, achieving one of the highest production rates recorded to date. The Co(Salen)-PIL demonstrates a syngas production rate of 168.1 mmol g−1 h−1, including a CO production rate of 69.3 mmol g−1 h−1, which is more than eight times higher than that of the best previously reported organic materials. Mechanistic investigations reveal that pyridine ions facilitate electron transfer from the heptazine light-harvester to the Co(Salen) active site. This study lays the groundwork for developing high-performance catalysts for photocatalytic syngas production.
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VACUUM
·
2025
·
IF 3.9
Jingwen Meng,Xiaoli Jin,Mengyuan Zhao,Zhuohua Chen,Weixi Hao,Shilong Lin,Xin Li,Fengyun Su,Fei Li,Kaiting Yang,Xiongtao Lv,Xuhan Zhang,Haiquan Xie
Limited light absorption and low carrier separation efficiency remain major obstacles to converting CO 2 into solar fuel. Rational design of semiconductor photocatalysts with unique structures holds promise for overcoming these challenges. In this study, Bi 4 O 5 Br 2 photocatalyst with a hollow core-shell architecture is synthesized via a one-step solvothermal method. This innovative structure facilitates efficient reflection and absorption of incident light within its internal cavity, while also minimizing the charge transfer path. Consequently, it significantly improves both light harvesting capabilities and charge carrier separation efficiency. Compared to the solid Bi 4 O 5 Br 2 (CO, 0.21 μmol g −1 h −1 ; CH 4 , 0.78 μmol g −1 h −1 ) and hollow Bi 4 O 5 Br 2 (CO, 0.25 μmol g −1 h −1 ; CH 4 , 0.99 μmol g −1 h −1 ) counterparts, the hollow core-shell Bi 4 O 5 Br 2 exhibits superior CO 2 photoreduction performance, achieving production rates of 3.61 and 2.40 μmol g −1 h −1 for CO and CH 4 , respectively. Notably, it also enhances C 2 H 4 production during the CO 2 reduction process, with a yield of 0.17 μmol g −1 h −1 , whereas no detectable C 2 H 4 is produced by either the solid or hollow Bi 4 O 5 Br 2 structures. This research provides fresh insights into the structural design of advanced photocatalysts and holds significant implications for converting CO 2 into high-value chemicals.
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2016
·
IF 1.207
Xiaoqing Wang,Libo Li,Jiangfeng Yang,Jinping Li
Two isomeric metal–organic frameworks (MOFs) with 2-dimensional (2D) and 3-dimensional (3D) topologies both comprised of Cu(II) and OTf (OTf = trifluoromethanesulfonate) ions were synthesized and characterized. The CO 2 , CH 4 and N 2 adsorption properties of the two isomeric MOFs were investigated from 263 K to 298 K at 0.1 MPa. The results showed that the 2D MOF exhibited a higher selectivity for CO 2 from CO 2 /CH 4 and CH 4 from CH 4 /N 2 compared to the 3D MOF, even though it possessed a lower surface area and pore volume. The higher adsorption heats of gases on the 2D MOF inferred the strong adsorption potential energy in the layered MOFs. Dynamic separation experiments using CO 2 /CH 4 and CH 4 /N 2 mixtures on the two MOFs proved that the 2D MOF had a longer elution time than the 3D MOF as well as better separation abilities.
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JOURNAL OF POROUS MATERIALS
·
2016
·Vol. 24
·期 3
·591-599
·
IF 1.385
Li Yanyan,Na Wei,Wang Hua,Gao Wengui
A series of Au–CuO/SBA-15 catalysts with 1–3 wt% Au and 30 wt% CuO were successfully prepared for CO 2 hydrogenation to methanol by chemical reduction and the following impregnation. The influence of Au content on the physicochemical properties of Au–CuO/SBA-15 catalysts was investigated in terms of ICP-AES, N 2 physisorption, XRD, TEM, N 2 O titration, XPS and H 2 –TPR technique. The results showed that the as-prepared Au–CuO/SBA-15 catalysts exhibited higher catalytic activity than CuO/SBA-15 catalyst. 2 % Au–CuO/SBA-15 catalyst showed the best catalytic activity with 13.5 % methanol selectivity and 24.2 % CO 2 conversion for CO 2 hydrogenation to methanol. The addition of Au NPs played an important role in improving the catalytic activity for CO 2 hydrogenation to methanol, which may be attributed to the interaction between Au and CuO.
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ChemSusChem
·
2016
·Vol. 9
·期 8
·806-812
·
IF 7.116
Qiwei Yang,Zhiping Wang,Zongbi Bao,Zhiguo Zhang,Yiwen Yang,Qilong Ren,Huabin Xing,Sheng Dai
Graphical Soak it up : The electrostatic environment around amine groups in ionic liquids (ILs) has critical influence on their CO 2 absorption mechanism, which enables the achievement of higher CO 2 capacity by tuning the local structure around the amine. Moreover, this work indicates that the actual CO 2 absorption mechanism by amino-acid ILs goes beyond the apparent CO 2 /amine stoichiometry. The last decade saw an explosion of interest in using amine-functionalized materials for CO 2 capture and conversion, and it is of great importance to elucidate the relationship between the molecular structure of amine-functionalized materials and their CO 2 capacity. In this work, based on a new quantitative analysis method for the CO 2 absorption mechanism of amino-acid ionic liquids (ILs) and quantum chemical calculations, we show that the small difference in the local structure of amine groups in ILs could lead to much different CO 2 absorption mechanisms, which provides an opportunity for achieving higher CO 2 capacity by structure design. This work revealed that the actual CO 2 absorption mechanism by amino-acid ILs goes beyond the apparent CO 2 /amine stoichiometry; a rigid ring structure around the amine group in ILs creates a unique electrostatic environment that inhibits the deprotonation of carbamic acid and enables actually equimolar CO 2 /amine absorption.
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JOURNAL OF THERMAL ANALYSIS AND CALORIMETRY
·
2017
·Vol. 131
·期 2
·1499-1507
·
IF 1.953
Lyu Jiaxun,Hu Dongdong,Liu Tao,Zhao Ling
The non-isothermal curing kinetics of epoxy resin system consisting of diglycidyl ether of bisphenol A (DGEBA) and m-xylylenediamine (MXDA) were investigated by high-pressure differential scanning calorimetry at different heating rates of 5, 10, 15 and 20 K min −1 under compressed carbon dioxide (CO 2 ) of 0.1–8 MPa. The activation energies were determined by isoconversional Kissinger–Akahira–Sunose method and Vyazovkin numerical method, and the average values decreased from 53.5 to 46.8 and 54.1 to 44.5 kJ mol −1 , respectively, when the CO 2 pressure increased from 0.1 to 8 MPa. It is indicated that the curing reaction of epoxy resin occurs more easily under higher-pressure CO 2 due to the promoted molecular movement, especially in the supercritical state. The non-isothermal curing kinetics were investigated by n th-order model and two-parameter autocatalytic model (Šesták–Berggren model), and the latter one analyzed by Málek method exhibited good agreement with the experimental data except the initial and final stages of the curing reaction.
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POLYMER
·
2016
·
IF 3.586
Jin Wang,Hongming Zhang,Yuyang Miao,Lijun Qiao,Xianhong Wang,Fosong Wang
UV-curable waterborne polyurethanes (CO 2 -UV-WPUs) with CO 2 -polyols as soft segment were firstly synthesized. In addition to the good mechanical performance, the coexistence of carbonate and ether moieties in soft segment assured the excellent hydrolysis resistance of CO 2 -UV-WPU compared with polybutylene adipate glycol based waterborne polyurethane (PBA-UV-WPU). Its retention of tensile strength reached 88% after 15 h immersion in 1.5% sodium hydroxide solution, while that of PBA-UV-WPU completely lost its mechanical property. The double bond density primarily governed the mechanical performance of CO 2 -UV-WPU, when it increased from 0.93 mmol/g to 2.4 mmol/g, the tensile strength increased from 29 MPa to 67 MPa, while elongation at break decreased from 150% to 9.6%, accompanied by the reduction of maximum water swelling percentage from 26.7% to 14.5%. The introduction of CO 2 -polyol as soft segment not only created a route to produce UV-curable waterborne polyurethane from CO 2 , but also provided polyurethane with novel value-added performance like good hydrolysis resistance. Moreover, the thermal/mechanical performance and hydrophilicity of CO 2 -UV-WPUs could be conveniently adjusted by controlling molecular weight of CO 2 -polyols, ensuring the application feasibility of CO 2 -UV-WPU.
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ACS Applied Materials & Interfaces
·
2017
·
IF 7.504
Shiming Zhang,Dingguan Wang,Qianhao Pan,Qinyuan Gui,Shenglong Liao,Yapei Wang
Solid materials for CO2 capture and storage have attracted enormous attention for gaseous separation, environmental protection, and climate governance. However, their preparation and recovery meet the problems of high energy and financial cost. Herein, a controllable CO2 capture and storage process is accomplished in an emulsion-templated polymer foam, in which CO2 is breathed-in under dark and breathed-out under light illumination. Such a process is likely to become a relay of natural CO2 capture by plants that on the contrary breathe out CO2 at night. Recyclable CO2 capture at room temperature and release under light irradiation guarantee its convenient and cost-effective regeneration in industry. Furthermore, CO2 mixed with CH4 is successfully separated through this reversible breathing in and out system, which offers great promise for CO2 enrichment and practical methane purification.
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APPLIED ORGANOMETALLIC CHEMISTRY
·
2012
·Vol. 26
·期 11
·600-603
·
IF 2.061
Dongsheng Bai,Huanwang Jing,Guangjian Wang
The synthesis of cyclic carbonates from epoxides and carbon dioxide catalyzed by cyanocobalamin and n -Bu 4 NI system was achieved under 0.8 MPa CO 2 pressure at 140°C without organic solvents. Propylene carbonate was obtained in 99% yield within 6 h under the optimized reaction conditions. The cyanocobalamin catalyst could be recycled with water and retained moderate catalytic activity. Copyright © 2012 John Wiley & Sons, Ltd.
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GREEN CHEMISTRY
·
2015
·Vol. 18
·期 2
·524-530
·
IF 8.02
Jin Wang,Hongming Zhang,Yuyang Miao,Lijun Qiao,Xianhong Wang,Fosong Wang
Carbon dioxide based oligo(carbonate–ether) diols (CO2-polyols) with both carbonate units and ether units in one polymer chain were prepared by copolymerization of CO2 and propylene oxide (PO) using a zinc–cobalt double metal complex as the catalyst, and used to prepare CO2 based waterborne polyurethanes (CO2-WPUs). The carbonate units in CO2-polyols improved the mechanical and oxidation resistance properties of CO2-WPUs, while the ether units in CO2-polyols enhanced the hydrolysis resistance of CO2-WPUs. The tensile strength of CO2-WPUs didn't show any obvious drop during immersion in a 0.25% sodium hydroxide solution, whereas that of oligoesterol based WPUs dropped over 50% after 300 min, and lost their mechanical properties after 520 min of immersion. Meanwhile, the retention of the tensile strength of the CO2-WPUs was ca. 72% even after 46 h of immersion in a 6 wt% H2O2 solution, while it was only ca. 32% for the oligoetherol based WPUs. Moreover, the thermal–mechanical performance of CO2-WPU films can be conveniently improved by adjusting the carbonate unit content (CU%) in CO2-polyols, i.e. when CU% in CO2-polyol increased from 30% to 66%, the glass transition temperature (Tg) increased from −7.8 °C to 18.8 °C, accompanied by an increase of tensile strength from 35.6 MPa to 52.2 MPa, and a decrease of elongation at break from 630% to 410%. This work suggests that the CO2-WPU may be a promising alternative to conventional WPU whose oligoetherol and oligoesterol were from fossil resources, and its comprehensive hydrolysis/oxidation resistance may be a bonus unavailable from common oligomerol based WPUs.
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CARBON
·
2013
·
IF 5.868
Xiangqian Fan,Lingxia Zhang,Guobin Zhang,Zhu Shu,Jianlin Shi
Nitrogen-doped microporous carbons were fabricated by a simple chemical activation strategy in which chitosan and K 2 CO 3 were employed as the precursor and activation agent, respectively. The textural and chemical properties of the porous carbons could be easily tuned by changing the ratio of K 2 CO 3 /chitosan and activation temperature. Due to their large pore volume , well-defined microporosity and relatively high nitrogen content, these porous carbons were applied as adsorbents for CO 2 capture and demonstrated excellent CO 2 uptake performances. In particular, the sample prepared at 635 °C with K 2 CO 3 /chitosan ratio = 2 shows a CO 2 uptake as high as 3.86 mmol g −1 at 25 °C, 1 atm. Furthermore, the CO 2 uptake remains almost constant in five consecutive adsorption–desorption cycles, indicating this material has great stability and recyclability as a CO 2 sorbent . In addition, an extraordinary separation selectivity against N 2 (CO 2 /N 2 selectivity of ca. 21) was also observed.
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