CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Pengchao Zang,Jiyun Tang,Yihui Tao,Hao Zhang,Xiaozhe Wang,Lin Cui,Shouyan Chen,Pei Zhao,Yong Dong
Calcium looping (CaL) represents a promising technology for CO 2 capture from flue gas. Nevertheless, CaO-based sorbents, characterized by high theoretical absorption capacities and low costs, experience significant degradation in CO 2 capture capacity during continuous cycling. In the present study, a novel K 2 CO 3 -doped CaO sorbent was synthesized through a concurrent hydrophilic impregnation process, and the performance of consecutive cyclic CO 2 capture was evaluated. The optimal 0.05 K-CaO demonstrated the highest CO 2 sorption (12.4 mmol/g), maintaining about 64 % of the initial sorption after 20 repetitive cycles under N 2 calcination atmosphere, which is 6.6 times greater than that of CaO. These findings indicated that K 2 CO 3 can regulate the particle size and the state of surface oxygen species in CaO-based sorbents while simultaneously enhancing CO 2 diffusivity on the sorbent surface. The DFT calculations indicated that the incorporation of K 2 CO 3 improved the mechanism of CaO chemisorption of CO 2 . Additionally, the vacancies and CO 3 2– generated by K 2 CO 3 doping can enhance the CO 2 sorption energy and reduce the system’s energy level. Notably, the net charge transfer for CO 2 sorption from K 2 CO 3 doping is greater than that from pure CaO, and the O atoms on the surface of K 2 CO 3 -CaO (001) exhibit strong covalent interactions with the C atoms in CO 2 , both of which facilitate CO 2 chemisorption. This study offers a comprehensive theoretical mechanism for the incorporation of K-based alkali metals to enhance the CO 2 capture performance of CaO sorbents.
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ACS Applied Nano Materials
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2024
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IF 5.3
Guoshu Deng,Guangze Nie,Xuehui He,Lin Li,Zhenkun Sun,Lunbo Duan
Conversion of CO2 into value-added chemicals is regarded as an effective way to reduce carbon emissions and improve the carbon recycling economy. In the process of hydrogenation of CO2 to CH4, nickel (Ni) has been extensively investigated due to its promising activity and easy availability. However, the inferior performance at low temperatures of Ni-based catalysts and the tendency of sintering at high temperatures lead to a rapid decline in activity, which hinders their large-scale applications. In this study, mesoporous silicas with highly ordered mesoporous structures but different pore symmetries and textural properties have been investigated as supports to synthesize Ni-based catalysts modified by La2O3. The effect of mesoporous symmetries and textural properties of the silica support on catalytic performance has been reasonably revealed. The catalysts supported on optimized silica with bicontinuous three-dimensional cubic pore symmetry exhibit considerably enhanced activity and stability in long-term CO2 methanation, which is attributed to the high dispersion of metal particles and the better mass transfer performance of interconnected mesopores in the silica support.
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Journal of Energy Chemistry
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2024
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IF 14
Baofei Sun,Wei Chen,Yanyi Huang,Daofu Wu,Heng Luo,Faguang Kuang,Hongmei Ran,Yichen Liu,Liqin Gao,Jinchen Zhou,Bo Gao,Qiang Huang,Xiaosheng Tang
Metal halide perovskites (MHP) are potential candidates for the photocatalytic reduction of CO 2 due to their long photogenerated carrier lifetime and charge diffusion length. However, the conventional long-chain ligand impedes the adsorption and activation of CO 2 molecules in practical applications. Here, a ligand modulation technology is employed to enhance the photocatalytic CO 2 reduction activity of lead-free Cs 2 AgInCl 6 microcrystals (MCs). The Cs 2 AgInCl 6 MCs passivated by Oleic acid (OLA) and Octanoic acid (OCA) are used for photocatalytic CO 2 reduction. The results show that the surface defects and electronic properties of Cs 2 AgInCl 6 MCs can be adjusted through ligand modulation. Compared with the OLA-Cs 2 AgInCl 6 , the OCA-Cs 2 AgInCl 6 catalyst demonstrated a significant improvement in the catalytic yield of CO and CH 4 . The CO and CH 4 catalytic yields of OCA-Cs 2 AgInCl 6 reached 171.88 and 34.15 µmol g −1 h −1 which were 2.03 and 12.98 times higher than those of OLA- Cs 2 AgInCl 6 , and the total electron consumption rate of OCA-Cs 2 AgInCl 6 was 615.2 µmol g −1 h −1 which was 3.25 times higher than that of OLA-Cs 2 AgInCl 6 . Furthermore, in situ diffuse reflectance infrared Fourier transform spectra revealed the enhancement of photocatalytic activity in Cs 2 AgInCl 6 MCs induced by ligand modulation. This study illustrates the potential of lead-free Cs 2 AgInCl 6 MCs for efficient photocatalytic CO 2 reduction and provides a ligand modulation strategy for the active promotion of MHP photocatalysts.
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FOOD RESEARCH INTERNATIONAL
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2024
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IF 7
Dongzhu Huang,Chenyi Sun,Yuhan Wu,Fangling Zheng,Qiqi Yang,Xinmeng Zhang,Qianying Dai,Xiaochun Wan,Qi Chen
This study aimed to investigate the effect of the combination of shaking and various anaerobic treatments on the aroma quality of gabaron oolong tea (GAOT) by chemical and sensory evaluation. The results showed that elevated anaerobic treatment harmed GAOT aroma, emphasizing undesirable attributes such as earthy, fatty, etc. A total of 85 volatiles were identified by gas chromatography-ion mobility spectrometry (GC-IMS), and the relationship between aroma attributes and volatiles were revealed by PLS regression projection and correlation network. Hexanal and octanal at inappropriate concentrations were main causes to the earthy attribute, while nonanal exhibited a potential masking effect against unpleasant attributes. Addition experiments and σ-τ plot analysis verified these associations. Furthermore, observing dynamic patterns of content changes of these three aldehydes in fresh leaves prior to tea thermal processing, providing references for future process optimization. These results provide a new direction for enhancing the quality of GAOT.
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PubMed
高影响因子
JOURNAL OF MOLECULAR LIQUIDS
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2024
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IF 5.3
Nan He,Qicheng Chen,Shan Cong,Nan An,Jing Fan,Fenhong Song,Xiwu Zhang
The absorption and separation of CO 2 is one of the main strategies to reduce carbon emissions and mitigate global climate change. In this context, a series of ternary superbase/betaine-based deep eutectic solvents (DESs) were synthesized to capture CO 2 , and their density, viscosity and thermal stability were investigated. The effects of temperature, pressure, different hydrogen bond donors (HBDs) and alkalinity of the superbase on their CO 2 affinity were evaluated by the isovolumetric saturation method. The uptake of CO 2 by the DES synthesized from betaine, 1,2-propanediol and 1,8-diazabicyclo(5.4.0)undec-7-ene reached a maximum of 1.5071 mol·kg −1 at 303.15 K and a pressure of 0.187 MPa. The simultaneous chemical and physical adsorption of CO 2 by the ternary DESs was verified by FTIR spectroscopy, and the absorption mechanism was also proposed. The reaction equilibrium thermodynamic model (RETM) was improved to obtain the “Active DES” model, which was correlated with the experimentally determined CO 2 solubility. The reaction equilibrium constants and Henry's law constants were obtained for each ternary system. The ternary superbase/betaine DESs proposed in this paper are green, economical and high-performance absorbers for capturing CO 2 .
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DYES AND PIGMENTS
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2024
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IF 4.1
Ji Xiong,Ming-Hui Chen,Xiang-Yu Li,Quan Shi,Yun-Hao Xu,Ya-Qing Feng,Bao Zhang
The sunlight-driven CO 2 fixation into high value-added industrial products constitutes a promising approach to mitigating global warming, offering an alternative to traditional thermally-driven fixation requiring high temperature and/or high pressure. Herein, we design and synthesize four isostructural porphyrinic covalent triazine frameworks ( Por-CTFs ) including metal-free Por-CTF ( H2Por-CTF ) and metallized Por-CTFs ( MPor-CTFs , M = Co, Zn, Cu) and their photocatalytic activity in CO 2 cycloaddition. All Por-CTFs exhibit wide light adsorption range in visible region via introducing porphyrins into the covalent triazine frameworks (CTFs) skeleton. Different metal ions which are well anchored in the MPor-CTFs skeleton not only offer Lewis acidic sites for substrate interaction but also apparently endow photocatalysts with longer photogenerated carrier lifetimes and higher electron-hole separation efficiency. Encouragingly, under visible light-assisted and mild conditions, the CoPor-CTF exhibits excellent photocatalytic performance achieving a reaction rate of 62.22 mmol g −1 h −1 , which is among the state-of-the-art cases for photocatalytic CO 2 cycloaddition and outperforms two other MPor-CTFs . This work demonstrates that the photophysical and electronic properties of Por-CTFs can be rationally tuned by incorporating various metal ions into porphyrin units to achieve effective photocatalysts for CO 2 cycloaddition.
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Nature Communications
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2025
·Vol. 16
·期 1
·1-18
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IF 15.7
Shen Yan,Fang Nan,Liu Xinru,Ling Yu,Su Yuming,Tan Tian,Chen Feng,Lin He,Zhao Boxuan,Wang Jin,Si Duanhui,Xie Shunji,Wang Ye,Zhou Da,Zhang Teng,Cao Rong,Wang Cheng
Interphases are critical in electrochemical systems, influencing performance by controlling ion transport and stability. This study explores a metal-organic interphase in the electrocatalytic reduction of CO 2 (CO 2 RR) on Cu, extending the concept of interphases to CO 2 conversion. Investigating organic modifications on CuO x , we discover metal-organic interphases over 10 nm thick in highly ethanol-selective systems, contrary to the expected monolayer adsorption. Using an automated platform, 1080 CO 2 RR experiments with 180 molecular modifiers identify functional groups affecting selectivity for ethanol and multi-carbon (C 2+ ) products. We find that these modifiers consistently produce metal-organic interphases on the Cu or CuO x surface. These interphases modulate Cu coordination, CO 2 RR intermediates, and interfacial water configuration, significantly improving electrocatalytic performance. Testing across 11 CuO x -based catalysts validates this approach, culminating in the development of two electrocatalysts that achieve ~80% faradaic efficiency for C 2+ products with ethanol partial current densities up to 328 and 507 mA cm −2 . This study highlights the pivotal role of interphases in CO 2 RR, advancing CO 2 conversion technologies.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Yanduo Liu,Mengwei Li,Jianing Guo,Ge Jin,Yue Yin,Yu Cui,Tong Sun
Recently, there has been a significant increase in interest in using photocatalysis for the energy conversion of polluting gases. In this research, sodium and ruthenium bimetallic functional sites co-modified bismuth tungstate (Ru/Na-Bi 2 WO 6 ) nanoflower photocatalyst was synthesized via the hydrothermal method. The CO 2 reduction products on the Bi 2 WO 6 substrate were CO (1.66 μmol/g/h, 68 %) and CH 4 (0.78 μmol/g/h, 32 %). After optimization, a significant change in the CO 2 products of the Bi 2 WO 6 -based composite material was observed, with CO (0.61 μmol/g/h, 3.6 %) and CH 4 (16.1 μmol/g/h, 96.4 %). Results showed that the dominance of CH 4 as the main product in the Ru/Na-BWO system is attributed to the effective doping of Na, which generates impurity energy levels composed of oxygen vacancies, lowering the conduction band position of Bi 2 WO 6 , thereby suppressing CO generation, and enhancing CH 4 selectivity by changing the CO 2 activation pathway. The remarkable performance is ascribed to the synergized adsorption and activation of CO 2 by the tandem Na + sites and Ru 0 sites. Specifically, the doped Na + sites play a major role in promoting the adsorption CO 2 molecules, while the Ru 0 sites play a dominant role in facilitating the activation of the intermediates.
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FUEL
·
2024
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IF 6.7
Yiming Chen,Chuan Wang,Qianwen Zhang,Ling Zhou,Yi Zhang
Methane synthesis derived from CO 2 hydrogenation has attracted great attention in terms of CO 2 recycling while suffering from the loss and sintering of active nickel species. Hence, we synthesized the Ni@Beta (Si/Al = 40) catalyst with a specific encapsulated structure by a simple hydrothermal synthesis using conventional Ni/SiO 2 as a unique silicon source. Compared to the conventional Ni/SiO 2 and Ni/Al 2 O 3 , the Ni@Silicalite-1 and Ni@Beta with encapsulated structures showed better stability. In addition, the Ni@Beta simultaneously exhibited the highest CO 2 conversion (74.2 %) and methane selectivity (93.5 %). All obtained catalysts were characterized by BET, ICP- OES, XRD, SEM-EDS, HRTEM, H 2 -TPR, CO 2 -TPD, in situ XPS, in situ DRIFTS, and NAP-XPS. Compared with the Ni@Silicalite-1 (Al-free zeolite), the aluminum-containing zeolite frameworks of the Ni@Beta got more electrons from the nickel active phases, so the metal-support interaction on the Ni@Beta was stronger, which was favorable for the stability of the Ni 0 phase. In addition, the Al-containing zeolite frameworks of the Ni@Beta inhibited the formation of volatile metal–molecule intermediates (gaseous Ni(CO) x ), which prevented serious sintering and loss of the nickel species. The in situ DRIFTS and NAP-XPS results not only successfully unveiled that the main reaction pathway was a formate route, but also showed that the Ni@Beta had the strongest capacity to adsorb and convert CO 2 , so it had the highest methanation activity.
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JOURNAL OF MEMBRANE SCIENCE
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2025
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IF 9
Zhongcheng Yang,Yue Yang,Yunna Li,Junwen Qi,Zhigao Zhu,Yujun Zhou,Jiansheng Li
A novel hollow fiber membrane containing a carbon-coated CuO x (CuC-HFM) was prepared for in-situ CO 2 electrochemical reduction to ethanol during wastewater treatment. The ratio of Cu-based metal organic framework/carbon black of 1/1 was relatively optimal (Cu 1 C 1 -HFM) due to higher pure water permeance (24.62 L m −2 h −1 bar −1 ), better hydrophilicity (contact angle of 60.00°), and more ethanol yield (165.22 mg L −1 m −1 ) at −2.5 V with KOH as electrolyte. For control group (Cu 2 C 1 -HFM and Cu 1 C 2 -HFM), they were 76.50°/89.10°, 3.90/4.42 L m −2 h −1 bar −1 , 64.85/57.32 mg L −1 m −1 , respectively. The peaks of Cu (002) crystal plane, Cu 2+ electronic orbits, covalent bonds between C and O, and CuO x were appeared on prepared membrane. The CuO x could strongly adsorb CO and subsequently carbon shell could selectively produce HOCCH and HOCHCH, which were benefit for CO 2 electro reduction to ethanol. Therefore, the Cu 1 C 1 -HFM owned higher ethanol production (88.50 g L −1 m −2 h −1 ) during filtrating anaerobic supernatant. Meanwhile, the membrane could reject 97.2 % COD with only 14.7 % membrane flux loss. The membrane without bias suffered 27.1 % flux loss. This system gave a new thought for CO 2 electro reduction and the CuC-HFM had a promising employment in anaerobic bioreactor in the future.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2024
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IF 8.1
Yajing Hu,Yong Men,Shuyi Xu,Yuanfen Feng,Jinguo Wang,Kaijie Liu,Yibo Zhang
Constructing the interface of Ni/Y 2 O 3 heterogeneous catalyst is a feasible strategy for efficient catalyst design in CO 2 methanation, which can create the active Y–O–Ni interfacial sites by utilizing the interaction between Ni and Y 2 O 3 . In this work, the strategy of using different nickel precursors (nickel nitrate, nickel acetate, basic nickel carbonate and nickel citrate) was used to prepare various Ni-based catalysts supported on Y 2 O 3 , which were estimated for their catalytic performance on CO 2 methanation. The catalysts were characterized based on BET, XRD, TEM, H 2 -TPR, XPS and CO 2 -TPD, etc. The results indicated a close correlation between the metal dispersion and particle size of Ni/Y 2 O 3 catalysts and the nickel precursor employed. The Y–O–Ni interface structure in Ni/Y 2 O 3 catalysts, associated with basic sites, provides a richer source of basic sites, offering more active sites for CO 2 adsorption and activation. Ni/Y 2 O 3 catalyst prepared with nickel nitrate as the precursor exhibited characteristics such as a highly enhanced nickel dispersion, a smaller nickel particle size, and more abundant metallic Ni 0 sites. Moreover, nickel nitrate-derived Ni/Y 2 O 3 catalyst exhibited optimal catalytic activity, achieving a CO 2 conversion rate of up to 92 % at 300 °C, with 100 % selectivity to CH 4 , and displaying good stability over 30 h. Therefore, the dispersion of Ni and the size of Ni particles could be controlled by adjusting the precursor, which is closely associated with the catalytic activity of Ni/Y 2 O 3 catalyst. This work unveils the interface-property relationship of Ni/Y 2 O 3 catalysts and provides a new insight into strategy of constructing more effective Ni-based catalyst for CO 2 methanation through the controlled nickel precursor.
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Chemical Engineering and Processing-Process Intensification
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2018
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IF 2.826
Dong-dong Hu,Jia-xun Lyu,Tao Liu,Mei-dong Lang,Ling Zhao
The solvation effect of compressed CO 2 on the curing reaction process of epoxy resin was investigated by using the in-situ FTIR. The isothermal curing kinetic constant and activation energy of diglycidyl ether of bisphenol A (DGEBA) with m-xylylenediamine (MXDA) was calculated via Kamal autocatalytic model. The autocatalyzed rate constants and activation energy under 0.1 MPa CO 2 are 0.7139 min −1 and 50.83 kJ/mol at 393 K, while those under 18 MPa CO 2 are 1.0928 min −1 and 36.36 kJ/mol, respectively. The increased kinetic constant and reduced activation energy suggests that the plasticization effect of CO 2 eases the chain movement, promotes the curing of epoxy resin, and increases the final conversion at relatively low temperature. Then, an amended Kamal model involving the diffusion factor was applied to better describe the curing process, which suggests that the high pressure CO 2 plays an important role to reduce the mass transfer resistance and intensify the curing process. Meanwhile, the activation energy determined by the isoconversional method, also decreases with CO 2 pressure at the same conversion. Especially, the activation energy at 90% conversion under 0.1 and 18 MPa CO 2 are 46.52 and 36.19 kJ/mol, respectively, which further confirms the solvation effect of CO 2 accelerates the curing of epoxy resin.
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危险品化学品经营许可证（带存储）