Reaction Chemistry & Engineering
·
2024
·Vol. 10
·期 1
·203-213
·
IF 3.4
Ning Ma,Liu Yang,Zhenchang Fang,Kaijia Jiang,Xinling Li,Zhen Huang
Deficiencies such as high viscosity, volatility, and rich phase precipitation limited the engineering application of non-aqueous absorbents. A series of high boiling point solvent screening experiments were conducted to develop an absorption saturated solution with a homogeneous phase at low viscosity (14.71 mPa s) in this study. Further addition of polyamines increased the absorption capacity by 42% (3.55 mol CO2 per kg). The 13C NMR results indicated that in the DETA/MEA/NMF blended amine system, MEA was involved in the deprotonation process of DETA zwitterions as proton acceptors. Quantum chemical calculations were utilized to compare the energies of each possible single-step reaction, providing insights into the reaction pathways of the blended amine system. The rate constant of the MEA/CO2 reaction was found to be 1.98 times that of the DETA/CO2 reaction, indicating lower reaction activity, consistent with NMR results. In addition, the results of the analysis of weak interactions revealed that the hydrogen bonds were key factors affecting the viscosity change and precipitation in non-aqueous absorbents, providing a new method for designing novel low-viscosity non-aqueous absorbents. The combination of theoretical analysis and experimental results underscores the potential of the blended amine non-aqueous absorbent as a feasible alternative for the industrial applications of CO2 capture.
研究领域:
化学工程
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
Advanced Science
·
2022
·Vol. 9
·期 16
·2105292
·
IF 17.521
Yawen Jiang,Xinyu Wang,Delong Duan,Chaohua He,Jun Ma,Wenqing Zhang,Hengjie Liu,Ran Long,Zibiao Li,Tingting Kong,Xian Jun Loh,Li Song,Enyi Ye,Yujie Xiong
Structural reconstruction is a process commonly observed for Cu-based catalysts in electrochemical CO 2 reduction. The Cu-based precatalysts with structural complexity often undergo sophisticated structural reconstruction processes, which may offer opportunities for enhancing the electrosynthesis of multicarbon products (C 2+ products) but remain largely uncertain due to various new structural features possibly arising during the processes. In this work, the Cu 2 O superparticles with an assembly structure are demonstrated to undergo complicated structure evolution under electrochemical reduction condition, enabling highly selective CO 2 -to-C 2+ products conversion in electrocatalysis. As revealed by electron microscopic characterization together with in situ X-ray absorption spectroscopy and Raman spectroscopy, the building blocks inside the superparticle fuse to generate numerous grain boundaries while those in the outer shell detach to form nanogap structures that can efficiently confine OH − to induce high local pH. Such a combination of unique structural features with local reaction environment offers two important factors for facilitating C−C coupling. Consequently, the Cu 2 O superparticle-derived catalyst achieves high faradaic efficiencies of 53.2% for C 2 H 4 and 74.2% for C 2+ products, surpassing the performance of geometrically simpler Cu 2 O cube-derived catalyst and most reported Cu electrocatalysts under comparable conditions. This work provides insights for rationally designing highly selective CO 2 reduction electrocatalysts by controlling structural reconstruction.
研究领域:
材料科学
·
电化学
·
环境科学
✓ 已验证
DOI
高影响因子
ACTA PHYSICO-CHIMICA SINICA
·
2016
·Vol. 32
·期 3
·605-610
·
IF 0.844
CHEN Feng-Feng,DONG Yan,SANG Xiao-Yan,ZHOU Yan,TAO Duan-Jian
Four tetrabutylphosphonium carboxylate ionic liquids ([P4444][CA]) were prepared, and their densities, viscosities, refractive indices, and conductivities were measured and correlated with thermodynamic and empirical equations in the temperature range of 298.15-348.15 K.
The influence of temperature on these four properties of [P4444][CA] was discussed, and their thermal expansion coefficient values were calculated. The CO2 absorption capacity of [P4444][CA] was studied at 313.15 K and 100 kPa. The results indicated that [P4444][Buty]
had the highest CO2 capture capacity among these ionic liquids, with an absorption capacity of 0.4 mol·mol-1 and balance time of less than 5 min.
研究领域:
化学工程
·
环境科学
✓ 已验证
DOI
高影响因子
Advanced Energy Materials
·
2019
·Vol. 9
·期 18
·1900364
·
IF 24.884
Chenyan Guo,Peng He,Rongrong Cui,Qi Shen,Nianjun Yang,Guohua Zhao
Electrochemical CO 2 reduction (ECCO 2 R) requires electrons, for example, from oxygen evolution reaction (OER). However, such a multiple-electron-involved reaction is complicated and kinetically slow, leading to high overpotential. Herein, OER is replaced with photoelectrocatalytic phenol oxidation reaction (PECPOR) that provides electrons for ECCO 2 R. In an integrated cell, ECCO 2 R is conducted on the cathode of Cu nanowires and PECPOR is performed on the anode of SnO 2 and Sb coated TiO 2 nanotubes. Significant improvement of ECCO 2 R into CO and hydrocarbons is realized when PECPOR is conducted at a high current density. The use of this integrated system results in the reduction of the specific energy consumption by a factor of 51.33%, compared with the utilization of two half-cells for individual ECCO 2 R and PECPOR. This study thus proposes a novel strategy to couple ECCO 2 R with PECPOR and eventually to tackle the problems of environmental pollution and energy crisis.
研究领域:
环境科学
·
电化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
VACUUM
·
2024
·
IF 3.8
Kaiting Yang,Xiongtao Lv,Jingwen Meng,Huiqing Wang,Lin Guo,Xin Li,Fengyun Su,Qing Lan,Zhengdao Li,Wei Wang,Yuwei Guo,Xiaoli Jin,Haiquan Xie
Photothermal catalytic reduction of CO 2 into high value-added C 2 hydrocarbon products is a promising method for efficient CO 2 conversion. However, current photocatalysts still encounter obstacles including limited photoabsorption range, rapid recombination of photogenerated carriers , and inadequate surface active sites. Herein, Bi 4 O 5 Br 2 co-modified with oxygen vacancy (OV) and metal bismuth (Bi) (Bi 4 O 5 Br 2 -OV@Bi) has been prepared to optimize these crucial issues. Bi 4 O 5 Br 2 -OV@Bi delivers a remarkably improvement in CO 2 photothermal conversion, reflecting by the notable increase in C 1 (CO and CH 4 ) and newly generated C 2 (C 2 H 4 and C 2 H 6 ) products compared to pristine Bi 4 O 5 Br 2 . In situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) spectrometry reveals that OC−COH* intermediate promotes the C–C coupling for produce C 2 hydrocarbons. This study strengthens the understanding of metal modification and defect engineering for forming C 2 hydrocarbons on bismuth-based photocatalysts .
研究领域:
材料科学
·
环境科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
·
2024
·Vol. 35
·期 11
·1-17
·
IF 2.8
Pan Deng,Wang Yanan,Lin Liwei,Zhang Yuzhe,Zhou Man,Li Zhongyu,Xu Song
Photothermal catalytic CO 2 reduction can combine photocatalysis and thermal catalysis by using full-spectrum solar energy to convert CO 2 into high value-added chemicals. This can effectively alleviate the problems of excessive CO 2 emissions and thermal catalytic energy waste. In this paper, a novel catalyst was prepared using Ce-MOF as a precursor to generate Cu/Ni/CeO 2 for efficient reduction of CO 2 to CO by hydrogenation. Due to the rod-like structure of CeO 2 and the high dispersion of Cu and Ni nanoparticles, 10%Cu 5%Ni CeO 2 can achieve a catalytic activity of 54.21 mmol g −1 h −1 in the full solar spectrum. The supported Cu and Ni metals are the active sites for catalytic reduction. Meanwhile, Cu and Ni enhanced the light absorption ability of the catalyst and the surface temperature under illumination. This is due to the hot charge carriers generated by LSPR effect in Ni and Cu metal nanoparticles, which can dissipate energy through local heating, thus increasing the temperature of the catalyst under illumination. It can be found that the CO 2 reduction activity of photo-assisted thermocatalysis is higher than that of thermal catalysis under the same conditions. Therefore, the combined effect of the electrons generated by UV–Vis light and the heating effect of near-infrared light on catalyst could improve the catalytic activity. This work might provide a potential strategy for efficient photothermal reduction of CO 2 in the future.
研究领域:
化学工程
·
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
INORGANIC CHEMISTRY
·
2024
·
IF 4.3
Di Li,Qin Li,Yimeng Zhou,Qiong Zhang,Qianjin Ye,Ran Yang,Deli Jiang
Steering selectivity in photocatalytic conversion of CO2, especially toward deep reduction products, is vital to energy and environmental goals yet remains a great challenge. In this work, we demonstrate a facet-dependent photocatalytic selective reduction of CO2 to CH4 in Cu-doped TiO2 catalysts exposed with different facets synthesized by a topological transformation from MIL-125 (Ti) precursors. The optimized round cake-like Cu/TiO2 photocatalyst mainly exposed with the (001) facet exhibited a high photocatalytic CO2 reduction performance with a CH4 yield of 40.36 μmol g–1 h–1 with a selectivity of 94.1%, which are significantly higher than those of TiO2 (001) (4.70 μmol g–1 h–1 and 52.6%, respectively), Cu/TiO2 (001 + 101) (18.95 μmol g–1 h–1 and 69.6%, respectively), and Cu/TiO2 (101) (14.73 μmol g–1 h–1 and 78.9%, respectively). The results of experimental and theoretical calculations demonstrate that the Cu doping dominating the promoted separation and migration efficiencies of photogenerated charges and the preferential adsorption on (001) facets synergistically contribute to the selective reduction of CO2 to CH4. This work highlights the significance of synergy between facet engineering and ion doping in the design of high-performance photocatalysts with respect to selective reduction of CO2 to multielectron products.
研究领域:
材料科学
·
环境科学
·
能源科学
✓ 已验证
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Guiming Xie,Xingyang Bai,Yanrui Niu,Runduo Zhang,Jian Liu,Qingyuan Yang,Zhou-Jun Wang
Making use of novel materials to develop efficient catalysts is one of the research hotspots for CO2 hydrogenation to methanol. Herein, UiO-66, a typical Zr-MOF, was modified by ethylene diamine tetraacetic acid (EDTA) to serve as a substrate for the synthesis of AuCu bimetallic catalysts. The resultant AuCu@UiO-66-EDTA catalyst exhibited a superior methanol production rate, which delivered a high space-time yield of methanol (3.34 gMeOH gmetal–1 h–1) at 250 °C and 3.0 MPa. The EDTA modification was found to effectively confine AuCu nanoparticles inside the framework of MOFs, which significantly reduced the metal particle size and enriched the oxygen vacancy concentration. As a consequence, more active sites were generated for methanol synthesis. Moreover, the AuCu@UiO-66-EDTA catalyst yielded more favorable reaction intermediates that could be converted to methanol at a faster rate. This work develops unique MOFs-encapsulated bimetallic catalysts and illuminates the positive effect of confinement.
研究领域:
材料科学
·
催化化学
✓ 已验证
DOI
PubMed
高影响因子
ACS Applied Polymer Materials
·
2025
·
IF 4.7
Yanling Liu,Xiao Peng,Yuan Li,Fei Wang,Xue Ai,Yuxi Huang,Xin Sun,Jie Zhao,Kai Li
Membrane separation technology has garnered significant attention for CO2 separation and purification, with mixed matrix membranes (MMMs) emerging as promising candidates due to their advantages of ease of processing, high mechanical strength, and thermal stability. The development of effective fillers for separation performance becomes one of the key foci in this area. In this work, CC3, a type of porous organic cages (POCs), was synthesized and functionalized with two amino-containing materials of different chain lengths. Polyethylenimine (PEI) and diethylenetriamine were used as modification agents to successfully graft amino groups onto the CC3 crystals to form defect-free Pebax mixed matrix membranes containing amino-functionalized CC3. The special porous structure of CC3 increases the gas permeability of the mixed matrix membrane by providing extra channels for the transportation of CO2. Besides, amino groups on functionalized CC3 interact with the chains of Pebax through hydrogen bonding, thus improving the compatibility between filler and matrix. The amino groups can further facilitate the transport of gases across the membrane through reversible reactions with CO2, which is further enhanced under humid conditions. Under optimal conditions, at 1 bar and 30 °C, the CO2 permeability of Pebax/PEI@CC3-MMMs was 342.33 Barrer with a selectivity of 33.38, while Pebax/DETA@CC3-MMMs exhibited a CO2 permeability of 273.34 Barrer and a selectivity of 35.77. This work demonstrates that amino-functionalized POCs (CC3) can effectively enhance the CO2 permeability and the CO2/N2 selectivity, which may provide a way to develop high-performance mixed matrix membranes with superior separation properties.
研究领域:
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
Journal of CO2 Utilization
·
2024
·
IF 7.2
Zhenrong Zheng,Junjie Dong,Jian Wang,Hongyang Wang
The majority of conventional flame retardants are made by chemical processes using petroleum resources, which cause serious pollution and waste of resources in the ecological environment. In this paper, flame retardants such as L-aspartic acid, DL-serine, L-tyrosine, L-lysine, L-phenylalanine, L-histidine, L-tryptophan, and glycine were employed to finish poly-(ethylene terephthalate) (PET) fabrics with supercritical CO 2 fluid. Scanning electron microscope (SEM) and Energy dispersive spectroscopy (EDS) were used to examine. the microstructure and chemical composition of flame-retardant PET fabrics. The limiting oxygen index (LOI) test and the vertical combustion test were used to assess the flame-retardant qualities of PET fabrics. Differential scanning calorimetry (DSC) and thermogravimetric analysis (TGA) were used to test and assess the thermal properties of PET fabrics. The strength test was used to assess the mechanical properties of PET fabrics. The results showed that the amino acid flame retardants were successfully finished on the PET fabrics by supercritical CO 2 (SC-CO 2 ) technology and improved the thermal stability of the PET fabric. In comparison to untreated PET fabric, the elongation at break was 13–15 % greater, and the breaking strength was not reduced. Among them, the PET fabrics treated with L-aspartic acid and L-lysine had better flame-retardant performance, there were no droplets, the LOI values were greater than 30 %, and the char length was less than 10 cm. After 45 minutes of soaping and 3 times of washing, the LOI values were still above 28 %, and there were no droplets. Therefore, the PET fibers treated with amino acids using SC-CO 2 technology effectively improved the flame-retardant performance of PET fabrics.
研究领域:
材料科学
·
纺织工程
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2020
·
IF 16.683
Xianying Wang,Yingshu Wang,Meichao Gao,Jinni Shen,Xipeng Pu,Zizhong Zhang,Huaxiang Lin,Xuxu Wang
Construction of composite semiconductors is an effective solution to elevate the efficiency of photocatalysis by prolonging lifetime of photogenerated hole and electrons. Herein, a heterojunction structure composite BiVO 4 /Bi 4 Ti 3 O 12 was synthesized via a facile in situ hydrothermal condition. The novel composite photocatalyst has excellent photocatalytic ability to reduce CO 2 with H 2 O into CH 3 OH and CO. The BiVO 4 /10 % Bi 4 Ti 3 O 12 sample shows the highest yields of CH 3 OH and CO up to 16.6 and 13.29 μmol g −1 h −1 , which was 12.39 and 5.68 times higher than that of pure BiVO 4 , and 9.88 and 2.80 times higher than that of pure Bi 4 Ti 3 O 12 , respectively. Such a high activity is attributed to the type II heterojunction structure which significantly enhances separation of photogenerated carriers and promotes collaboration between the water oxidation on the Bi 4 Ti 3 O 12 and the CO 2 reduction on BiVO 4 . The photocatalytic reaction mechanism of CO 2 on the composite was proposed according to experiment results.
研究领域:
材料科学
·
环境科学
·
化学工程
✓ 已验证
DOI
高影响因子
Nature Communications
·
2025
·Vol. 16
·期 1
·1-10
·
IF 15.7
Song Zhilong,Fan Linfeng,Lu Shuaihua,Ling Chongyi,Zhou Qionghua,Wang Jinlan
Directly generating material structures with optimal properties is a long-standing goal in material design. Traditional generative models often struggle to efficiently explore the global chemical space, limiting their utility to localized space. Here, we present a framework named Material Generation with Efficient Global Chemical Space Search (MAGECS) that addresses this challenge by integrating the bird swarm algorithm and supervised graph neural networks, enabling effective navigation of generative models in the immense chemical space towards materials with target properties. Applied to the design of alloy electrocatalysts for CO 2 reduction (CO 2 RR), MAGECS generates over 250,000 structures, achieving a 2.5-fold increase in high-activity structures (35%) compared to random generation. Five predicted alloys— CuAl, AlPd, Sn 2 Pd 5 , Sn 9 Pd 7 , and CuAlSe 2 are synthesized and characterized, with two showing around 90% Faraday efficiency for CO 2 RR. This work highlights the potential of MAGECS to revolutionize functional material development, paving the way for fully automated, artificial intelligence-driven material design.
研究领域:
材料科学
·
人工智能
·
化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）