SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Hong Zhu,Yan Huang,Simi Li,Lingkui Zhao,Junfeng Zhang
The most promising approach to tackling the greenhouse gases is CO 2 capture and storage (CCS), and amine solid adsorbents are the most widely investigated materials. In this work, Zr species as an accelerator promote CO 2 adsorption of the Pentatethylenehexamine (PEHA)/sepiolite (SEP) adsorbents. The adsorption rate, CO 2 adsorption capacity, and amine efficiency were significantly improved under various conditions (temperature, gas flow, and CO 2 concentration) by the introduction of the optimal content of Zr, the optimal HSEP-Zr 0.13 -PEHA 0.5 -600 adsorbent exhibited 1.80 mmol/g at 60 °C. Adsorption experiments combine with characterization (TG, XPS, NH 3 -TPD, SEM and TEM) exhibited that the introduction of Zr species were high dispersion on sepiolite, and Zr-O bond was formed in the structure of sepiolite. The acidity of the sepiolite supporter was enhanced by Zr which is benefit for amine loading. Above all resulted in the regeneration and thermal stability of the adsorbent were improved together. The economic evaluation results demonstrated that the adsorbent with Zr species is low-cost for large-scale post-combustion CO 2 capture.
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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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FUEL
·
2023
·
IF 7.4
Miaomiao Tan,Xiangyu Li,Yu Feng,Bing Wang,Lina Han,Weiren Bao,Liping Chang,Jiancheng Wang
The ordered mesoporous silica materials with large pore volume were prepared from the silica source extracted from fly ash by supercritical hydrothermal activation. This path has the advantages of low activation temperature, high silicon utilization, and matching of silicon source extraction and the hydrothermal synthesis process. The obtained mesoporous silica support was impregnated with 60 wt% tetraethylenepentamine (TEPA) to prepare excellent solid amine sorbent. The thermogravimetric results showed that the CO 2 adsorption capacity of sorbent could reach 5.17 mmol/g under 75 °C and dry pure CO 2 atmosphere. At the same time, the sorbent had fast adsorption kinetics (5.08 mmol/g in 10 min) and stable cycle performance. Consequently, the obtained sorbent is a promising candidate for carbon capture technologies.
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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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Journal of Physical Chemistry C
·
2023
·
IF 3.7
Zesheng Deng,Jiazhen Cao,Songchang Hu,Shiqun Wu,Mingyang Xing,Jinlong Zhang
CO2 photoreduction is considered one of the potential ways to achieve carbon neutralization since it uses green solar energy without introducing additional carbon sources during the process of converting CO2 to fuels. However, limited light utilization and poor charge separation often give rise to undesirable CO2 photoreduction performance. Herein, a generic approach using carbon spheres as templates to construct transition metal oxides with multishelled hollow structures is reported. The multishelled hollow structure has been proven to be efficient for improving CO2 photoreduction. Furthermore, we constructed a Z-scheme heterojunction photocatalyst (CdS/Au/ZnCrO4) through introducing CdS into a multishelled hollow ZnCrO4 sphere with Au nanoparticles as a charge transfer medium. Benefiting from the multishelled hollow structure’s induced light utilization and large surface area and Z-scheme heterojuncion promoted charge separation, a high CO production of 2.95 μmol g–1 h–1 was achieved on CdS/Au/ZnCrO4 without using any sacrificial agents, which was 18.4 times and 24.6 times higher than that of CdS and ZnCrO4. This work provides a generic method for constructing controllable multishelled hollow spheres and is expected to offer guidance for promoting CO2 photoreduction through structure regulation and heterojunction construction.
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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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Nature Communications
·
2023
·Vol. 14
·期 1
·1-13
·
IF 16.6
Sun Ji Wei,Wu Xuefeng,Liu Peng Fei,Chen Jiacheng,Liu Yuanwei,Lou Zhen Xin,Zhao Jia Yue,Yuan Hai Yang,Chen Aiping,Wang Xue Lu,Zhu Minghui,Dai Sheng,Yang Hua Gui
Practical electrochemical CO 2 -to-CO conversion requires a non-precious catalyst to react at high selectivity and high rate. Atomically dispersed, coordinatively unsaturated metal-nitrogen sites have shown great performance in CO 2 electroreduction; however, their controllable and large-scale fabrication still remains a challenge. Herein, we report a general method to fabricate coordinatively unsaturated metal-nitrogen sites doped within carbon nanotubes, among which cobalt single-atom catalysts can mediate efficient CO 2 -to-CO formation in a membrane flow configuration, achieving a current density of 200 mA cm −2 with CO selectivity of 95.4% and high full-cell energy efficiency of 54.1%, outperforming most of CO 2 -to-CO conversion electrolyzers. By expanding the cell area to 100 cm 2 , this catalyst sustains a high-current electrolysis at 10 A with 86.8% CO selectivity and the single-pass conversion can reach 40.4% at a high CO 2 flow rate of 150 sccm. This fabrication method can be scaled up with negligible decay in CO 2 -to-CO activity. In situ spectroscopy and theoretical results reveal the crucial role of coordinatively unsaturated metal-nitrogen sites, which facilitate CO 2 adsorption and key *COOH intermediate formation.
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CHEMBIOCHEM
·
2023
·Vol. 24
·期 10
·e202300114
·
IF 3.2
Bo-Yu Zhang,Zhen-Hua Wu,Zi-Yi Chu,Ke Li,Jia-Fu Shi
Graphical A monolithic catalyst of Filler-CA@Lys-HOF-1 (FCLH) was prepared by coating chemical sorption of CA on the surface of the filler followed by the coating of Lys-HOF-1. The highest catalytic activity of FCLH was obtained by regulating the amount of HOF-1 monomer added. Due to the protection of Lys-HOF-1, the FCLH showed good tolerance against acidity and salinity, which could retain about 80.2 % of the original activity after 9 h incubation in simulated seawater. The catalytic activity of FCLH could retain 85.4 % of the initial activity after 10 cycles. In short, we may offer a promising biocatalyst for carbon mineralization, which may drive down carbon emissions when used for CO 2 capture and conversion on offshore platforms. Exhausted emission of carbon dioxide (CO 2 ) from ships or offshore platforms has become one of the major contributors to global carbon emissions. Enzymes such as carbonic anhydrase (CA) have been widely used for CO 2 mineralization because of their high catalytic rate. However, CA in seawater is easy to inactivate and difficult to reuse. Immobilization would be a feasible solution to address the stability issue, which, however, may cause an increase of internal diffusion resistance and reduced catalytic activity. In this regard, design of high-performance biocatalysts for acquiring high catalytic activity and stability of CA is highly desirable. Herein, a monolithic catalyst of Filler-CA@Lys-HOF-1 (FCLH) was prepared by chemical sorption of CA on the surface of the Filler followed by the coating of Lys-HOF-1. The highest catalytic activity of FCLH was obtained by regulating the amount of HOF-1 monomer added. Due to the protection of Lys-HOF-1, the FCLH showed good tolerance against acidity and salinity, which could retain about 80.2 % of the original activity after 9 h incubation in simulated seawater. The catalytic activity of FCLH could retain 85.4 % of the initial activity after 10 cycles. Hopefully, our study can provide a promising biocatalyst for CO 2 mineralization, which may drive down carbon emissions when used for CO 2 capture and conversion on offshore platforms.
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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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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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