Nanoscale
·
2021
·Vol. 13
·期 28
·12157-12163
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IF 7.79
Kaixiang Shen,Qiang Wei,Xin Wang,Qiang Ru,Xianhua Hou,Guannan Wang,Kwan San Hui,Jiadong Shen,Kwun Nam Hui,Fuming Chen
Multifunctional electrocatalytic desalination is a promising method to increase the production of additional valuable chemicals during the desalination process. In this work, a multifunctional desalination device was demonstrated to effectively desalinate brackish water (15 000 ppm) to 9 ppm while generating formate from captured CO2 at the Bi nanoparticle cathode and releasing oxygen at the Ir/C anode. The salt feed channel is sandwiched between two electrode chambers and separated by ion-exchange membranes. The electrocatalytic process accelerates the transportation of sodium ions and chloride ions in the brine to the cathode and anode chamber, respectively. The fastest salt removal rate to date was obtained, reaching up to 228.41 μg cm−2 min−1 with a removal efficiency of 99.94%. The influences of applied potential and the concentrations of salt feed and electrolyte were investigated in detail. The current research provides a new route towards an electrochemical desalination system.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2021
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IF 3.764
Xiaoyan Pei,Jiang Liu,Weihao Rao,Xiantao Ma,Zhiyong Li
Carbon dots (CDs) have attracted great attention in recent years owing to their potential applications in such as photocatalysts, organic synthesis, and bioimaging. However, it is always difficult for the separation and recycling of carbon dots from homogeneous reaction systems, which may limit their application in catalysis. A stimuli-responsive phase transfer of CDs is promising to solve these problems. In this work, we developed a novel class of CO2-responsive carbon dots decorated with different molecular weight polyetheramines (PEAs) (Mn = 230, 400, 2000 g/mol, respectively) and investigated their phase transfer behavior. It was found that PEA230-CD were well able to reversibly transfer between water and organic solvents by alternative bubbling and removal of CO2, the phase transfer efficiency of PEA400-CD was about 40%, and PEA2000-CD cannot transfer. The mechanism of the CO2-switched phase transfer involves the reversible reaction of PEA-functionalized CDs with CO2 and reversible formation of hydrophilic bicarbonates salts. As an example of applications, the phase transfer strategy was successfully applied in a Henry reaction by using the CDs as catalysts for efficient homogeneous catalysis, heterogeneous separation, and recycling of the CDs.
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DALTON TRANSACTIONS
·
2019
·Vol. 49
·期 13
·3965-3969
·
IF 4.052
Suying Wang,Zhengwen Liu,Andrew T. Smith,Yanxian Zeng,Luyi Sun,Weixing Wang
Dry hydrated potassium carbonate (DHPC) is a free-flowing powder prepared by uniformly mixing hydrated K2CO3 and hydrophobic nanosilica. We demonstrated that DHPCs can absorb CO2 rapidly because of their high surface-to-volume ratio. Their CO2 capture performance is superior to that of 30 wt% monoethanolamine (MEA), an industry standard. DHPC-75 (containing 75 wt% K2CO3) has a CO2 uptake capacity of 233 mg g−1 (90% saturation uptake within 13 min), higher than the widely used 30 wt% MEA aqueous solution (111 mg g−1, 90% saturation uptake within 25 min). DHPC-75 also exhibits an excellent cycling performance, thus becoming a promising candidate for practical application.
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JOURNAL OF CATALYSIS
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2018
·
IF 6.759
Shao-Hong Guo,Jie Zhou,Xue Zhao,Chun-Yi Sun,Si-Qi You,Xin-Long Wang,Zhong-Min Su
Development of efficient, selective and low-cost photocatalysts, ideally constructed from Earth-abundant elements, is still a big challenge for CO 2 photoreduction. Herein, adopting mixed halides strategy, the activity of all-inorganic perovskites toward CO 2 reduction is enhanced sharply under simulated sunlight without photosensitizer, meanwhile maintaining high selectivity of CO and CH 4 production. Via regulating ratio of Br and Cl, the yield of CO and CH 4 changes obviously and the optimized catalyst is CsPb(Br 0.5 /Cl 0.5 ) 3 with a total yield of CO and CH 4 up to 875 μmol/g (selectivity of 99%) which outperforms any other reported halide perovskites and is 4.5 and 9.1 folds higher than that of CsPbBr 3 and CsPbCl 3 under the same condition. The efficient charge separation and moderate stability in mixed-halide perovskites may account for the excellent performance in CO 2 reduction. This study may provide a new strategy in design of high performance and low-cost halide perovskite materials for photocatalysis.
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PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
·
2024
·
IF 6.9
Zhongqing Shen,Zixian Jia,Kunpeng Yu,Jing Xie,Lijiao Qin,Lin Gao,Baozhong Li,Xuehai Wang,Jianzhong Yin
Depolymerization shows promise as a strategy for converting waste plastic into monomers that can be used for repolymerization. However, catalytic approaches would be more complex and expensive due to catalyst separation, recovery, and recycling. Here, we present a CO 2 -enhanced subcritical methanolysis method without catalyst that can generate monomer from poly(ethylene terephthalate)(PET). The synergistic effect of CO 2 on the subcritical methanolysis process for PET depolymerization was investigated including the CO 2 initial pressure, reaction temperature and reaction time. Under subcritical conditions, the optimal reaction parameters with PET conversion ratio of 100% and DMT yield of 79.1% are as follows: temperature of 220℃, methanol to PET mass ratio of 6:1 and reaction time of 50 min. Moreover, through the analysis of experimental data, it was concluded that the depolymerization reaction follows a first-order kinetics, with the reaction rate being 2–3 times faster than the traditional process. However, the apparent activation energy for both reactions is found to be similar, with values of 135.1 kJ·mol −1 and 146.2 kJ·mol −1 , respectively.
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iScience
·
2024
·
IF 4.6
Qun Fan,Guangxu Bao,Hai Liu,Yihan Xu,Xiaoyi Chen,Xiangrui Zhang,Kai Li,Peng Kang,Sheng Zhang,Xinbin Ma
Interfacial investigation for fine-tuning microenvironment has recently emerged as a promising method to optimize the electrochemical CO 2 reduction system. The electrical double layer located at the electrode-electrolyte interface presents a particularly significant impact on electrochemical reactions. However, its effect on the activity and selectivity of CO 2 electrocatalysis remains poorly understood. Here, we utilized two-dimensional mica flakes, a material with a high dielectric constant, to modify the electrical double layer of Ag nanoparticles. This modification resulted in a significant enhancement of current densities for CO 2 reduction and an impressive Faradaic efficiency of 98% for CO production. Our mechanistic investigations suggest that the enhancement of the electrical double layer capacitance through mica modification enriched local CO 2 concentration near the reaction interface, thus facilitating CO 2 electroreduction.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2024
·
IF 8.1
Wei Zhou,Mazhar Ahmed Memon,Mengmeng Niu,Xinqiang Fan,Yanan Jiang,Xian Zhang,Yuan Liu
Copper (Cu) based catalysts are frequently used in CO 2 hydrogenation, particularly in reverse water-gas shift (rWGS) and CO 2 -to-methanol reaction. Cu 0 and Cu + are the key species affecting the catalyst performance and product distribution . Therefore, constructing and adjusting Cu 0 /Cu + active pairs is significant for the catalyst design . In this study, Cu 0 /Cu + active pairs are obtained by utilizing the properties of perovskite-type oxides (PTOs). A series of CaTi 1-x Cu x O 3 and Ca 0.8 La 0.2 Ti 1-x Cu x O 3 (x = 0.05, 0.10, 0.15, 0.30, 0.40 and 0.50) were synthesized via citric acid complexing method and part of the Cu species entered the PTOs lattice. After reduction, large Cu particles and highly-dispersed Cu clusters were obtained simultaneously. The dispersed Cu clusters have more interfaces with the PTOs and provide abundant Cu + while large Cu particles tend to aggregate and supply mainly Cu 0 . Cu 0 activates H 2 and CO 2 and plays a vital role in the rWGS reaction . Cu + is the active site for methanol synthesis and it can strongly absorb CO. The ratio of Cu 0 /Cu + varies with different Cu content and doping La can also adjust the chemical state of surface Cu. The performance test demonstrates that both excessively high and low Cu 0 /Cu + ratios are beneficial for CO generation, while a moderate ratio is suitable for methanol synthesis . These insights provide a method for regulating the chemical state of surface metal species and help the catalyst design for CO 2 hydrogenation.
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APPLIED ENERGY
·
2017
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IF 7.182
Hongwei Li,Zhigang Tang,Zhimin He,Jingjie Cui,Dong Guo,Zhijun Zhao,Xian-zhong Mao
Diethyl succinate (DES) is a new and highly efficient carbon dioxide (CO 2 ) absorption solvent. Vapor-liquid equilibrium data for the CO 2 + DES system were obtained experimentally from 288.15 K to 318.15 K by the gas-phase recirculation method, and were modeled using the Kritchevsky-Kasarnovsky model and Peng-Robinson equation of state . The vapor-liquid equilibrium data of the DES system were compared with those of the diethyl carbonate (DEC) and dimethyl carbonate (DMC) systems, and Henry constant was found to follow DES < DEC < DMC. The absorbed and released energy as simulated using Gaussian 09 software shows that the CO 2 absorption capacity of DES is better than that of the DEC and DMC. A continuous absorption-desorption experimental setup was established for the CO 2 -DES system to determine the optimum operating conditions of a liquid-gas ratio of 1.337, an absorption temperature range from 291.15 to 293.15 K, a desorption temperature range from 433.15 to 443.15 K, and a nitrogen (N 2 ) flow of 0.5 NL/min. The DES system costs less than the DEC and DMC systems when using N 2 gas-stripping desorption. A novel desorption process with compression and condensation was used to regenerate solvent and to simplify the process. This system costs less than those for thermal desorption, and gas-stripping desorption. The results from the DES system were better than those of the DMC and DEC systems. DES shows potential as a CO 2 absorbent.
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Nature Communications
·
2025
·Vol. 16
·期 1
·1-10
·
IF 15.7
Chen Xiuling,Chen Guining,Xie Cong,Wu Lei,Liu Gongping,Li Nanwen,Jin Wanqin
High-performance gas separation membranes have potential in industrial separation applications, while overcoming the permeability-selectivity trade-off via regulable aperture distribution remains challenging. Here, we report a strategy to fabricate Polyolefin Reweaved Ultra-micropore Membrane (PRUM) to acquire regulable microporous channel. Specifically, olefin monomers are dispersed uniformly into a pristine membrane (e.g., PIM-1) via solution diffusion method. Upon controlled electron beam irradiation, the olefin undergoes a free radical polymerization, resulting in the formation of olefin polymer in-situ reweaved in the membrane. The deliberately regulated and contracted pore-aperture size of the membrane can be accomplished by varying the olefin polymer loading to achieve efficient gas separation. For instance, PIM-1 PRUM containing 27 wt% poly-glycidyl methacrylate demonstrate CO 2 permeability of 1976 Barrer, combined with CO 2 /CH 4 and CO 2 /N 2 selectivities of 58.4 and 48.3 respectively, transcending the performance upper bounds. This controllable and high efficiency-design strategy provides a general approach to create sub-nanometre-sized pore-apertures of gas separation membranes with wide universality.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Han Li,Yushan Li,Huailing Diao,Haipeng Ren,Jianming Chen,Jinfeng Wang,Qingtao Liu,Xungai Wang
Wild silk cocoons are light-weight composite structures with unique properties. One such property is the intriguing CO 2 gating property (i.e., unidirectional flow of CO 2 ) exhibited by the wild Antheraea pernyi ( A. pernyi ) silkworm cocoon. This study investigated the hierarchical structural and compositional features of A. pernyi cocoons and their impact on CO 2 adsorption. For the first time, soap-film flowmeter testing method and gas permeability testing method were used to quantitatively demonstrate the A. pernyi cocoons’ CO 2 adsorption property and selectivity for gas mixture. The results showed that the multi-layered composite structure of A. pernyi cocoons, coupled with calcium oxalate crystals, play a crucial role in their CO 2 adsorption and separation performance. These findings shed light on the unique functional design of wild silk cocoons and provide a new biomimetic approach for developing materials and structures to address global challenges such as CO 2 capture and storage.
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ENERGY & FUELS
·
2025
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IF 5.3
Yinchun Liang,Hongyu Duan,Weida Chen,Lihui Sun,Feng Zhang
New absorbents combining the advantages of phase separation and easily regenerated products were prepared with 2-methyl-2-amino-1-propanol (AMP) as the main absorbent and tertiary amines as the auxiliary absorbents and phase splitters. The absorption performances of absorbents containing different tertiary amines were systematically compared. Among these tertiary amines, N,N,N′,N′-tetramethyl-1,3-propanediamine (TMPDA) exhibited the most effective properties. For the absorbent TMPDA–AMP–H2O system (TAH), an absorption load of approximately 2.6 mol/kg was achieved. The kinetic and thermodynamic properties of TAH absorption were evaluated. It was found that the absorption products were readily decomposed into HCO3–, and the regeneration efficiency of TAH was above 91% at 358 K, while the regeneration energy consumption was only 2.0 GJ/t CO2. It should be noted that the addition of TMPDA effectively inhibited the precipitation of bicarbonate, thus leading to a higher absorption capacity and lower energy consumption per ton of CO2 loaded.
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Journal of Energy Chemistry
·
2024
·
IF 14
Qiong Rao,Yuanhui Shen,Ying Pan,Hongguang Jin
Repurposing of carbon dioxide to valuable chemicals and fuels with the assistance of renewable energy is essential for balanced carbon cycle. Here, a new CO 2 conversion strategy was demonstrated that utilized concentrated solar energy to directly drive chemical looping reverse water gas shift process, which simultaneously coupled the photothermal and photochemical effects to achieve enhanced CO 2 reduction reactivity and 100% CO selectivity. The solar-driven chemical looping CO 2 reduction on Ni-Fe 2 O 3 /La 0.8 Sr 0.2 FeO 3 exhibited great activity, with an average CO production rate of up to 0.28 mmol/g oc /min at 283 o C. The product yield of the solar-driven reaction was almost 600% higher than that of the thermal reaction at the same temperature. The CO production overcame the thermodynamic equilibrium limitation under the combined impact of thermal and non-thermal effects of direct-light illumination. Light irradiation reinforced reactive gas adsorption and dissociation of carbonate intermediates, and stimulated oxygen ion migration and lattice oxygen transformation, thus promoting the reactivity. The concept of concentrated solar energy to drive chemical looping reverse water gas shift opens a new avenue for effective CO 2 resource utilization and solar fuel production.
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