CATALYSIS TODAY
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2023
·
IF 5.3
Hangjie Li,Liang Wang,Feng-Shou Xiao
Cu/ZnO/Al 2 O 3 catalyst has been widely studied in the hydrogenation of CO 2 to methanol, but it still suffers from insufficient catalyst stability and methanol selectivity. Herein, we overcome these issues by introducing the silica promoter to the catalyst, achieving the Cu/ZnO/Al 2 O 3 /SiO 2 (CZAS) catalysts with significantly improved methanol selectivity and catalyst durability. Characterizations of samples showed that the silica species efficiently hindered the sintering of Cu nanoparticles during the catalysis, exhibiting constant performances in the continuous tests. In addition, the silica also electronically modulated the Cu nanoparticles that result in abundant Cu δ+ species in the catalyst, which minimized the methanol decomposition to improve the methanol selectivity, compared with the silica-free Cu/ZnO/Al 2 O 3 catalyst. As a result, the CZAS exhibited CO 2 conversion at 12.6 % and methanol selectivity at 85.1 %, giving a one-pass methanol yield at 10.7 %. The strategy in this work might provide an efficient route for enhancing the current industrial catalysts.
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ACS Sustainable Chemistry & Engineering
·
2023
·
IF 8.4
Yongping Gan,Min Huang,Fei Yu,Xing Yu,Zhanjun He,Jin Liu,Tiejun Lin,Yuanyuan Dai,Qiang Niu,Liangshu Zhong
Light-driven methane conversion to methanol with high selectivity is considered a challenging and promising reaction for sustainable development. Herein, Cu/CeO2 catalysts were prepared for photocatalytic methane conversion with CO2 as a soft oxidant. Methanol was the sole liquid product with a high selectivity of 96.2% and a high yield of 88.9 μmol g–1 h–1 for the 2Cu/CeO2 catalyst. Investigation of the structure–performance relationship indicated that oxygen vacancies facilitated the trapping of photogenerated electrons and avoided carrier recombination. In addition, as a soft oxidant, CO2 can also capture photogenerated electrons to be reduced to CO and further accelerate the formation of CH3OH. A catalytic mechanism study demonstrated that methane and hydroxyl were oxidized by photogenerated holes to •CH3 and •OH, respectively, and thus, methanol was generated through the combination of •CH3 and •OH.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Jinxian Feng,Junyan Li,Lulu Qiao,Dong Liu,Pengfei Zhou,Jun Ni,Hui Pan
Zn-based materials are regarded as a family of promising electrocatalysts for electrochemical CO 2 reduction reaction (e-CO 2 RR), especially for the CO 2 -to-CO conversion. However, their electrocatalytic performances should be improved and the conversion mechanism needs to be further studied. In this work, we fabricate Cu-incorporated ZnO (Cu 25 Zn-A) on Zn plate for e-CO 2 RR catalyst by a facile annealing method. We find that Cu 25 Zn-A achieves a high CO Faraday efficiency > 90% with a CO yield rate of 0.49 mmol cm −2 h −1 . The improved catalytic activity on Cu 25 Zn-A is mainly attributed to the Cu steps on the reconstructed surface in the reaction: (1) that weakens the OH - /CO 3 2- adsorption, leading to the anti-poisoning surface by preventing the formation of Zn hydroxide/carbonates; and (2) that enhances the adsorption/activation of reactants and stabilizes the intermediates. Additionally, the density of defects in Zn oxide is increased by the Cu-incorporation, resulting in improved deoxygenation step. Our findings may provide insightful understanding on the mechanism and guide the design of novel electrocatalyst for effective CO 2 reduction.
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CHEMICAL ENGINEERING SCIENCE
·
2023
·
IF 4.7
Qinghai Long,Shuo Wang,Shufeng Shen
Maintaining water balance in water-lean solvents is drawing special attention as it may affect the capture performance and process stability. In this study, novel water-lean solvents containing ethylene glycol monohexyl ether (EGHE) and secondary alkanolamines was proposed for energy-saving postcombustion CO 2 capture. Excess water from wet flue gas can be discharged from the desorber overhead condensate which can produce a spontaneous phase-separation feature. Less than 0.8 mass% EGHE was observed in the water-rich phase of the biphasic condensate. Effect of water content in these absorbents on CO 2 capture performance was discussed. Most notably, regeneration energy consumption increased significantly as increasing water content in the absorbent. The proposed water-lean absorbents with 10 % H 2 O can reduce the regeneration heat duty by about 40% in comparison with aqueous MEA, indicating that the novel water balance design can make it competitive in a practical sense.
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Small
·
2023
·Vol. 19
·期 27
·2207915
·
IF 13.3
Jinchen Zhou,Daofu Wu,Changqing Tian,Zhiyu Liang,Hongmei Ran,Bo Gao,Zhongtao Luo,Qiang Huang,Xiaosheng Tang
Lead halide perovskite materials have great potential for photocatalytic reaction due to their low fabrication cost, unique optical absorption coefficient, and suitable band structures. However, the main problems are the toxicity and instability of the lead halide perovskite materials. Therefore, a facile synthetic method is used to prepare lead-free environmentally friendly Cs 2 TiX 6 (X = Cl, Cl 0.5 Br 0.5 , Br) perovskite materials. Their structural and optical characteristics are systematically investigated. The band gaps of the produced samples are illustrated to be from 1.87 to 2.73 eV. Moreover, these materials can keep high stability in harsh environments such as illumination and heating, and the Cs 2 Ti(Cl 0.5 Br 0.5 ) 6 microcrystals demonstrate the yields of 176 µmol g −1 for CO and 78.9 µmol g −1 for CH 4 after light irradiation for 3 h, which is of the first report of Ti-based perovskite photocatalysts. This finding demonstrates that the Ti-based perovskites will create opportunities for photocatalytic applications, which may offer a new idea to construct low-cost, eco-friendly, and bio-friendly photocatalysts.
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Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Zhen Huang,Lingri Ying,Fengchun Gong,Jianfeng Lu,Weilong Wang,Jing Ding,Jinyue Yan
Carbon dioxide capture and storage (CCS) is considered as a promising strategy for reducing CO 2 emissions. However, the further development of CO 2 adsorption materials with high selectivity and high adsorption capacity is the top priority of this technology . In this study, we used the μ-OH sites of the MIL-125 metal–organic framework (MOF) to modify it with aminosilane to synthesize a new MOF adsorbent (SAP-MIL-125) with improved CO 2 adsorption capacity at room temperature. Although there are no open metal sites on the MIL-125 surface, it is possible to load aminosilanes onto it. Under the same adsorption conditions, the CO 2 adsorption by SAP-MIL-125 was significantly improved compared to that of the original MIL-125. Adsorption isotherm and kinetics models were used to clarify that the adsorption mechanism of CO 2 on SAP-MIL-125 was non-homogeneous layer chemisorption . SAP-MIL-125 has excellent selectivity toward CO 2 (compared to N 2 ) and good stability over five adsorption–desorption cycles. The adsorption of CO 2 by SAP-MIL-125 is a spontaneous exothermic process. An in-depth investigation of the adsorption mechanism suggests that the acid–base interactions of carbamates is the mechanism of CO 2 adsorption. Density functional theory and frontier molecular orbital calculations showed that the main adsorption sites for the modified adsorbent were nitrogen-containing groups on the surface of aminosilanes, with the primary amines having the highest affinity for CO 2 . In conclusion, a novel material modification method for MOFs is provided, which was used to fabricate a CO 2 adsorbent with great potential for development.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Yuchao Chen,Yubin Wang,Zifei Yan,Jian Deng,Guangsheng Luo
Efficient selective removal of H 2 S over CO 2 is the critical absorption process for the gas desulfurization in the petrochemical and refining industries. In this work, we tried to achieve high-selective removal of H 2 S from a mixed gas with CO 2 using a nonaqueous methyldiethanolamine solution in a membrane gas–liquid microdispersion microreactor. The influence of structural parameters and operation parameters on the removal efficiency of H 2 S and CO 2 were systematically investigated. In addition, the mechanism of selective absorption H 2 S over CO 2 was explained in detail. Furthermore, the selective absorption performance of the membrane microdispersion microreactor was compared with other devices. The results showed that the H 2 S removal efficiency and selective factor could be up to 99.4 % and 16.6, respectively. The selectivity factor of H 2 S to CO 2 in the membrane microdispersion microreactor is higher than that of most of reported devices. This work provides a promising selective absorption H 2 S device and technology for the process intensification of gas desulfurization.
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JOURNAL OF APPLIED POLYMER SCIENCE
·
2023
·Vol. 140
·期 33
·e54268
·
IF 3
Shoucun Zhang,Yujing Bian,Xueyin Yan,Guoli Fang,Shengwei Guo
The separation of the proteins is of great theoretical and practical importance for biotechnological application. Considering the requirement of non-destructive separation, the stimulus–response method is an alternative to the separation of protein. In this work, a cellulose-based composite with CO 2 stimulus–response property is prepared by a simple coprecipitation of poly ( N , N ˊ-diethylamino ethyl methacrylate)- co -poly (hydroxyethyl methacrylate) (PDH) and cellulose mixture solution. Subsequently, these composites as the adsorption medium are used to separate the bovine serum albumin (BSA, as the model protein) from solution through stimulus–response course (by CO 2 /N 2 alternation). The results indicate that the ratio of the copolymers/cellulose composite have an obvious effect on the separation of BSA. The average maximum adsorption capacity can get to 562.6 mg/g, and the composites exhibits good adsorption/desorption cycling characteristics. After the composite materials are cycled for three times, the adsorption capacity can still decrease to 300 mg/g. Due to its high adsorption capacity and low preparation cost, the composite is expected to be widely used in industry.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Haifei An,Weijian Tian,Xin Lu,Huanmei Yuan,Liyun Yang,Hao Zhang,Haoming Shen,Hao Bai
Adsorbents with high adsorption capacity and high selectivity are crucial for carbon capture, utilization and storage (CCUS) technology applied to industrial flue gas to reduce carbon emissions. In this paper, a defect-rich hierarchical porous Mg-MOF-74 was synthesized successfully with MgCl 2 ·6H 2 O used as a metal source considering that the weak coordination of Cl − may interfere with the normal coordination process of metal centers and organic ligands, which causes the formation of crystal defects. Through the analysis of a series of characterizations, ligand deletion of Mg-MOF-74 prepared with MgCl 2 ·6H 2 O was confirmed, and the deleted ligand was estimated to be approximately 20% compared with the traditional Mg-MOF-74 prepared with Mg(NO 3 ) 2 ·6H 2 O, which led to mesopores accounting for 36.9%, and the width of mesopores reached 13.1 nm. Compared with traditional Mg-MOF-74, the adsorption heat of CO 2 at zero load of the defect-rich hierarchical porous Mg-MOF-74 increased from 36 kJ·mol −1 to 46 kJ·mol −1 , and the saturated adsorption capacity of CO 2 under ambient pressure was improved by 15%. Interestingly, the IAST selective adsorption performance of CO 2 /N 2 was increased by 20 times. Compared with the saturated adsorption capacity for traditional Mg-MOF-74, the equivalent adsorption capacity of hierarchical porous Mg-MOF-74 only needs 17 kPa, indicating that it is suitable for carbon capture operation in a real flue environment. Calculations of density functional theory (DFT) confirmed that the active site of the hierarchical porous Mg-MOF-74 has a lower adsorption energy with CO 2 due to the presence of defects, which is regarded to play a key role in improving the CO 2 capture performance.
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JOURNAL OF MEMBRANE SCIENCE
·
2023
·
IF 9.5
Ning Li,Chao Ma,Mao Ye,Xiangyu Guo,Zhihua Qiao,Chongli Zhong
Mixed-matrix membranes (MMMs) have arisen as an energy-saving and efficient candidate for CO 2 separation that can mitigate the greenhouse effect. However, challenges still remain in achieving good filler-polymer compatibility and high separation performance. Herein, a mechanochemistry method is proposed to synthesize an amine-functionalized ultramicroporous ZIF-62 (ZIF-UC-6) with good CO 2 affinity. Amino functional groups and open metal sites are introduced into ZIF-UC-6, which significantly improve its CO 2 adsorption capacity of ZIF-62. According to the ideal adsorption solution theory (IAST) calculation, the CO 2 /CH 4 and CO 2 /N 2 selectivity of ZIF-UC-6 is ∼80 and ∼140, respectively. Besides, when ZIF-UC-6 is incorporated into Pebax, hydrogen bonds can form between filler and polymer, which can increase the interfacial compatibility in the MMMs. The optimized membrane possesses a CO 2 permeability of ∼560 barrer, together with high CO 2 /CH 4 and CO 2 /N 2 selectivity of 41.8 and 86.2, surpassing the corresponding upper bounds. Moreover, the prepared MMMs have good pressure resistance and long-term stability. This work demonstrates an effective route for developing MMMs with good interfacial compatibility and high CO 2 separation performance for potential industrial applications.
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Small
·
2023
·Vol. 19
·期 33
·2301498
·
IF 13.3
Ting Zhu,Sheng Wang,Zhiqian Yu,Hucheng Song,Jun Xu,Kunji Chen
Lithium-carbon dioxide (Li-CO 2 ) batteries have attracted much attention due to their high theoretical energy density. However, due to the existance of lithium carbonate and amorphous carbon in the discharge products that are difficult to decompose, the battery shows low coulombic efficiency and poor cycle performance. Here, by adjusting the adsorption of carbon dioxide (CO 2 ) on ruthenium (Ru) catalysts surface, this work reports an ultralow charge overpotential and long cycle life Li-CO 2 battery that consists of typical lithium metal, ternary molten salt electrolyte (TMSE), and Ru-based cathode. Experimental results show that the Ru catalysts deposited on quartz nanofiber (QF) can suppress the four-electron conversion of CO 2 to lithium carbonate (Li 2 CO 3 ). As a result, the battery shows a long-cycle-life of over 457 cycles at 1.0 A g −1 with a limited capacity of 500 mAh g −1 Ru . Remarkably, a recorded low discharge potential of ≈3.0 V has been achieved after 35 cycles at 0.5 A g −1 , with a charge potential retention of over 99%. Moreover, the battery can operate over 25 A g −1 and recover 96% potential. This battery technology paves the way for designing high-performance rechargeable Li-CO 2 batteries with carbon neutrality.
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Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Xin Fang,Chu-Ya Wang,Long-peng Zhou,Qi Zeng,Heng-Deng Zhou,Qi Wang,Guangcan Zhu
Photocatalytic reduction of CO 2 into valuable resources presents an efficient solution to mitigate the energy crisis and effects of climate change . However, the low efficiency of photocatalytic CO 2 reduction of photocatalysts under visible light irradiation limits their industrial applications. Bismuth oxybromide (BiOBr) is a typical visible-light-driven photocatalyst with an appropriate band gap, but the charge separation efficiency still needs to be improved. In this work, the Au-doped BiOBr nanosheets with enhanced electrochemical characteristics were successfully synthesized through a simple one-step hydrothermal procedure. After Au-doping modification, the charge separation efficiency of BOB-Au-I sample were measured as 2.5 times than that of BiOBr nanosheets. And the BOB-Au-I samples exhibited an outstanding photocatalytic capacity for converting CO 2 to CO with a yield rate of approximately four times higher than that of BOB nanosheets under visible light irradiation. Furthermore, the mechanism of CO 2 reduction was elucidated through in situ Fourier-transform infrared spectroscopy. This study provides a facile method for achieving Au-doping modification of BiOBr nanosheets for efficient reduction of CO 2 .
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