APPLIED CATALYSIS B-ENVIRONMENTAL
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2020
·
IF 16.683
Jia-Fang Xie,Jie-Jie Chen,Yu-Xi Huang,Xing Zhang,Wei-Kang Wang,Gui-Xiang Huang,Han-Qing Yu
In this work, a novel Cu-Pd heterostructure, derived from CuCl-PdO x hexagonal microplates, was prepared to tune selective single hydrocarbon production from electrochemical CO 2 reduction. The CuCl-PdO x hexagonal microplates were synthesized by a dual-potential electrodeposition technique, followed by electrochemical reduction to form Cu-Pd heterostructure. This Cu-Pd heterostructure exhibited a much higher CO 2 -to-CH 4 selectivity (32 % Faradaic efficiency, FE) compared to pure Cu or Pd. Moreover, Cu-Pd heterostructure showed excellent suppression on C 2 H 4 generation (below 1 % FE). The density functional theory calculations suggested that the hollow site of Pd region in the Cu-Pd heterostructure could stablize CO* intermediate and selectively lowered the energy demand for CH 4 formation rather than C 2 H 4 . This work provides new opportunities of designing Cu-based electrocatalysts for selective CO 2 reduction to single hydrocarbon.
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RSC Advances
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2020
·Vol. 10
·期 43
·25911-25917
·
IF 3.119
Xing Jiang,Yong Kong,Zhiyang Zhao,Xiaodong Shen
The objective of this research was to develop a novel spherical amine grafted silica aerogel for CO2 capture. A spherical silica gel was synthesized by dropping a sodium silicate based silica sol into an oil bath. Amine grafting was achieved by bonding 3-aminopropyltriethoxysilane onto the framework of the silica gel. The spherical amine grafted silica gels were dried using vacuum drying to prepare the spherical amine grafted silica aerogels (SASAs). The synthetic mechanism of the SASAs was proposed. The structures and the CO2 adsorption performances of SASAs were researched. The amine loading of the SASAs increased with the grafting time, however, the specific surface area and pore volume sharply decreased owing to the blockage of the pore space. Excess amine loading led to the decrease of the CO2 adsorption capacity. The optimal CO2 adsorption capacity was 1.56 mmol g−1 with dry 1% CO2 and at 35 °C. This work provides a low-cost and environmentally friendly way to design a capable and regenerable adsorbent material.
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Small
·
2023
·
IF 13.3
Fengwei Zhang,Han Zhang,Zhenhe Jia,Shuai Chen,Siming Li,Jijie Li,Wen-Yan Zan,Qiang Wang,Yawei Li
The transition metal–nitrogen–carbon (M─N─C) with MNx sites has shown great potential in CO 2 electroreduction (CO 2 RR) for producing high value-added C 1 products. However, a comprehensive and profound understanding of the intrinsic relationship between the density of metal single atoms and the CO 2 RR performance is still lacking. Herein, a series of Ni single-atom catalysts is deliberately designed and prepared, anchored on layered N-doped graphene-like carbon (x Ni 1 @NG-900, where x represents the Ni loading, 900 refers to the temperature). By modulating the precursor, the density of Ni single atoms ( D Ni ) can be finely tuned from 0.01 to 1.19 atoms nm −2 . The CO 2 RR results demonstrate that the CO faradaic efficiency (FE CO ) predominantly increases from 13.4% to 96.2% as the D Ni increased from 0 to 0.068 atoms nm −2 . Then the FE CO showed a slow increase from 96.2% to 98.2% at −0.82 V versus reversible hydrogen electrode (RHE) when D Ni increased from 0.068 to 1.19 atoms nm −2 . The theoretical calculations are in good agreement with experimental results, indicating a trade-off relationship between D Ni and CO 2 RR performance. These findings reveal the crucial role of the density of Ni single atoms in determining the CO 2 RR performance of M─N─C catalysts.
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FUEL
·
2023
·
IF 7.4
Mei Luo,Xiangmin Fu,Shuo Geng,Ziwei Li,Min Li
CO 2 electrocatalysis reduction (CO 2 RR) is considered to be one of the most efficient methods to achieve carbon neutralization and realize renewable energy conversion. Unfortunately, at present, CO 2 electrocatalysts confront the challenges of high overpotential, low selectivity, and poor stability. Ag based electrocatalysts are considered to be the most promising catalysts for CO production via CO 2 RR on a large scale, due to their relatively higher catalytic performance and more abundant reserves compared with other noble metals. Whereas, they still suffer from high cost. In this paper, we design bimetallic CuAg/CeO 2 -6 catalysts by the simple impregnation method for CO 2 RR, exhibiting the highest FE CO of 84% at –1.1 V vs. RHE compared with other bimetallic catalysts with different Cu/Ag ratio and monometal catalysts. XPS results demonstrate the electron delocalization effect not only between Cu and Ag bimetals but also among CeO 2 support. This effect results in the electronic structure change and the formation of the highest concentration of oxygen vacancies, promoting the CO 2 adsorption and activation as well as facilitating the formation of COOH* intermediates as evidenced by the in situ ATR-SEIRAS measurements. Additionally, the highest active surface for CO 2 RR and the smallest charge resistance of CuAg/CeO 2 -6 also contributes to its good CO 2 RR performance. This work sheds light on the design of other efficient CO 2 RR catalysts through electronic structure tuning by bimetallic strategy.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2023
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IF 4.2
Haiwei He,Chuigang Fan,Songgeng Li,Weigang Lin
Reductive decomposition of phosphogypsum for CaO production is proposed to proceed under a CO2 atmosphere to avoid the presence of CaS in the product. In combination with thermodynamic analysis, thermogravimetric tests are conducted with the monitoring of gas composition to explore the reaction mechanism between C/CaSO4 and CO2. Three reaction stages are identified, i.e., CaSO4 reduction, reaction of CaS with CaSO4, and CaS oxidation by CO2. The reaction path depends on the C/CaSO4 molar ratio and temperature. Further, phosphogypsum decomposition in CO2 is further conducted in a fluidized bed reactor, and data show that over 96.2% of CaSO4 in phosphogypsum is decomposed into CaO at 1000 °C and a C/CaSO4 molar ratio of 1.0 within 83.7 min. Phosphogypsum decomposition in air or nitrogen has lower CaO production. Further, kinetic analyses of CaS oxidation with CO2 in the presence of CaSO4 were performed to illustrate the effect of the CaS–CaSO4 reaction on the CaS–CO2 reaction.
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JOURNAL OF CATALYSIS
·
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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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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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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PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
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2024
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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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APPLIED ENERGY
·
2017
·
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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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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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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Results in Engineering
·
2025
·
IF 7.9
Ruiqi LI,Jie LING,Dongqiang LEI
The key to photocatalytic conversion of CO 2 is to improve the efficiency of solar energy utilization. Numerous studies have been devoted to modulating the forbidden bandwidth of photocatalytic materials, thereby altering the response of catalysts to light irradiation. In this paper, CO 2 conversion efficiency enhancement by photothermal catalytic means using precious metal-free LDHs@AC composites. The results show that photothermal catalytic conversion is 3.3 times more efficient than photocatalytic conversion in CO 2 conversion. The photocurrent transient response results show that the LDHs@AC material in the photothermal catalytic reaction, at higher experimental temperatures, the transfer of electrons from Ti 1 Li 3 Al 2 -LDHs to move the AC is faster, and the rate of the redox reaction is increased, which significantly improves the photocatalytic performance of the LDHs material.
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