INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2024
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IF 3.8
Li Wang,Zhangmiao Ye,Caihong Lin,Yugao Wang,Jinping Li,Jiangfeng Yang
N2O/CO2 separation in the tail gas of adipic acid presents a significant challenge due to the closely resembling physical characteristics exhibited by CO2 and N2O. Herein, adsorption and separation performances of CO2 and N2O on FAU-type zeolite Y with different cations (Na+ and Ag+) were studied comprehensively. After Ag+ exchange, zeolite Y changes from a CO2-selective adsorbent to a N2O-selective adsorbent. AgY shows high N2O uptake (95.7 cm3/g) but relatively low adsorption heat (23.1 kJ/mol), making it suitable for N2O/CO2 separation. In situ Fourier transform infrared spectrometry indicates that N2O is successfully adsorbed on AgY. The breakthrough experiment reveals that AgY exhibits superior performance in the separation of N2O/CO2 at a flow rate of 20 mL/min while also exhibiting a favorable retention time and ratio of retention time with CO2 breakthrough time, which can reach up to 4.1 min and 0.24, respectively, which makes it an optimum N2O/CO2 separation material reported so far.
研究领域:
化学工程
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材料科学
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DOI
高影响因子
CATALYSIS LETTERS
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2024
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IF 2.3
Yu Pengxin,He Jianshen,Du Mingzhi,Lai Ying,Peng Yang,Yu Fuqing,Wang Hongmin,Yang Weiran
Disproportionation of alcohols to the corresponding alkanes and aldehydes/ketones is an important reaction, especially for biomass valorisation. Previously, we reported for the first time that hydroiodic acid can be used as an efficient catalyst for the alcohol disproportionation reaction, and the interconversion between hydroiodic acid and iodine is the key step for hydrogen transfer. As a continuation of our previous work, this work mainly focused on the mechanistic study involved and studied the difference between hydroiodic acid or molecular iodine as the catalyst for the disproportionation of alcohols. Density Functional Theoretical calculation indicated the oxidation step was a synergistic reaction process through the iodine effect on oxygen-hydrogen bond, which was proved by the characteristic oxygen-iodine bond captured by in-situ Attenuated Total Reflectance Fourier Transform Infrared. A non-polar solvent was preferable for the reaction with iodine. Addition of small amount of water was shown to be beneficial for the reaction, because water promoted Brønsted acidity of hydroiodic acid and accelerated the rate-determining step. Finally, we showed that the system was also applicable to various benzyl, allyl alcohols, and some heterocyclic alcohols. Graphical Abstract
研究领域:
化学
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催化反应机制
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产品关联
DOI
高影响因子
Gels
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2023
·Vol. 9
·期 5
·392
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IF 4.6
Huaiyuan Dou,Quan Ye,Yan He,Xuemin Cui
Lithium batteries, as energy storage devices, are playing an increasingly important role in human society. As a result of the low safety of the liquid electrolyte in batteries, more attention has been paid to solid electrolytes. Based on the application of lithium zeolite in a Li-air battery, a non-hydrothermal conversed lithium molecular sieve was prepared. In this paper, in-situ infrared spectroscopy, together with other methods, was used to characterize the transformation process of geopolymer-based zeolite. The results showed that Li/Al = 1.1 and 60 °C were the best transformation conditions for the Li-ABW zeolite. On this basis, the geopolymer was crystallized after 50 min of reaction. This study proves that the formation of geopolymer-based zeolite occurs earlier than the solidification of the geopolymer and shows that the geopolymer is a good precursor for zeolite conversion. At the same time, it comes to the conclusion that the formation of zeolite will have an impact on the geopolymer gel. This article provides a simple preparation process for lithium zeolite, explores the preparation process and mechanism, and provides a theoretical basis for future applications.Keywords:in-situ infrared spectroscopy;non-hydrothermal transportation;Li-geopolymer;Li-ABW
研究领域:
材料科学
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能源化学
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产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Lixiong Xu,Yifan Yang,Chenyue Li,Rongqian Ning,Jun Ma,Mengqin Yao,Shuo Geng,Fei Liu
The electrocatalytic glycerol oxidation reaction (GOR) is an efficient way to reduce the overpotential of the anodic reaction of electrocatalytic water splitting with abundant high-value byproducts. However, it has always been difficult to reveal a clear reaction path and real active site during the electrocatalytic glycerol oxidation reaction (GOR) process. In this work, NiOOH/Ni 3 S 2 /NF, a model catalyst was synthesized by the two-step method, and the reaction path of the electrocatalytic oxidation of glycerol on NiOOH/Ni 3 S 2 /NF was clearly unveiled by the in situ infrared and Raman analysis. In addition, the TEM after GOR and in-situ Raman intuitively demonstrated that the NiOOH was the real active site during the GOR process. Consequently, the synthesized NiOOH/Ni 3 S 2 /NF catalyst achieved a current density of 10 mA cm −2 at 1.227 V vs . RHE and obtained a high formic acid Faraday efficiency of 97.7 % at a low potential of 1.4 V vs . RHE. This work demonstrates an effective method for unveiling the GOR mechanism and the other relevant electrocatalytic reaction processes.
研究领域:
电化学
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催化科学
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产品关联
DOI
高影响因子
Catalysts
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2021
·Vol. 11
·期 6
·710
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IF 4.146
Linmeng Huo,Tian Wang,Keng Xuan,Lei Li,Yanfeng Pu,Chenxin Li,Congzhen Qiao,Hao Yang,Yan Bai
The adsorption and activation of both CO2and methanol are mainly affected by the distance of the Lewis acid site, Zr4+, and Lewis base, Zr4+/O2−, of the Zr-based catalysts. In this paper, Zr-incorporated SBA-15 (Zr-SBA-15) and Zr-grafted SBA-15 (Zr/SBA-15) catalysts were prepared with different Zr environments, and were analyzed with N2adsorption–desorption isotherms, X-ray diffraction, UV-vis spectra, and XPS. It was proposed that Zr-SBA-15 catalyst with Si-O-Zr-OH and Zr-O-Si-OH structure exhibited non-adjacent sites between Zr4+and Zr4+/O2−, while Zr/SBA-15 catalyst with Zr-O-Zr-OH structure showed neighboring sites between Zr4+and Zr4+/O2−. Furthermore, the Zr/SBA-15 catalyst exhibited good catalytic activity, while no DMC was detected over the Zr-SBA-15 catalyst at the same reaction conditions. For combined in situ infrared and catalytic performance, it was indicated that the methanol and CO2could be activated to form DMC, only when the Zr4+and Zr4+/O2−sites existed and were adjacent to each other in the Zr-O-Zr-OH of Zr/SBA-15 catalyst.Keywords:dimethyl carbonate;in situ FTIR spectra;ZrO2-grafted SBA-15;Zr-incorporated SBA-15;carbon dioxide
研究领域:
催化化学
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环境科学
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DOI
高影响因子
Journal of the American Chemical Society
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2024
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IF 14.4
Ernest Pahuyo Delmo,Yian Wang,Yihua Song,Shangqian Zhu,Haichuan Zhang,Hongming Xu,Tiehuai Li,Juhee Jang,Yongjun Kwon,Yinuo Wang,Minhua Shao
The reaction mechanism of CO2 electroreduction on oxide-derived copper has not yet been unraveled even though high C2+ Faradaic efficiencies are commonly observed on these surfaces. In this study, we aim to explore the effects of copper anodization on the adsorption of various CO2RR intermediates using in situ surface-enhanced infrared absorption spectroscopy (SEIRAS) on metallic and mildly anodized copper thin films. The in situ SEIRAS results show that the preoxidation process can significantly improve the overall CO2 reduction activity by (1) enhancing CO2 activation, (2) increasing CO uptake, and (3) promoting C–C coupling. First, the strong *COO– redshift indicates that the preoxidation process significantly enhances the first elementary step of CO2 adsorption and activation. The rapid uptake of adsorbed *COatop also illustrates how a high *CO coverage can be achieved in oxide-derived copper electrocatalysts. Finally, for the first time, we observed the formation of the *COCHO dimer on the anodized copper thin film. Using DFT calculations, we show how the presence of subsurface oxygen within the Cu lattice can improve the thermodynamics of C2 product formation via the coupling of adsorbed *CO and *CHO intermediates. This study advances our understanding of the role of surface and subsurface conditions in improving the catalytic reaction kinetics and product selectivity of CO2 reduction.
研究领域:
材料科学
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电化学
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催化反应
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产品关联
DOI
PubMed
高影响因子
Environmental Science-Nano
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2024
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IF 5.8
Jingwei Hong,Wanli Li,Jin Shang,Hiromi Yamashita,Yun Hu
Utilizing electrocatalysis to convert CO2 into high-value industrial raw materials can not only effectively reduce CO2 emissions but also achieve a closed carbon cycle. This method holds great potential for addressing global warming and alleviating the fossil fuel crisis. Here, we report a novel electrocatalyst for CO2 reduction composed of a composite material derived from Cu-MOF74 and Cu2O, synthesized under the regulation of an appropriate amount of KOH. The research results indicate that the unique Cu0/Cu+ interface in Cu-MOF74/Cu2O-350 enhances the adsorption of reaction intermediates, providing more active sites for CO2 reduction. Additionally, the moderate carbonization during the thermal treatment process increases conductivity and enriches the electrochemical active surface area, accelerating the charge transfer rate. Consequently, this composite exhibits excellent CO2 reduction performance. At -1.3 V vs. RHE, the Faraday efficiency (FE) for C2H4 production reached up to 32.48%, which was significantly higher than that of pure Cu2O-350 (9.25%) and Cu-MOF74-350 (15.52%). Even after 6 hours of reaction, the FE for C2H4 remained above 24.52%, reflecting its good stability. Furthermore, we utilized in-situ infrared spectroscopy to study the key intermediates of the relevant reduction products, inferring the possible reaction pathways for the formation of HCOOH and C2H4. This study provides a simple synthesis method for the preparation of high-selectivity MOF-derived composite catalysts for the electrocatalytic reduction of CO2 to value-added chemicals.
研究领域:
电化学
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材料科学
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环境科学
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催化
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产品关联
DOI
高影响因子
ACS Catalysis
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2022
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IF 13.7
Xiwen Song,Chengsheng Yang,Xianghong Li,Zhongyan Wang,Chunlei Pei,Zhi-Jian Zhao,Jinlong Gong
Understanding the nature of adsorbates and intermediates on catalytic surfaces is critical for the development of highly efficient systems for CO2 conversion. However, the role of structural hydroxyl groups in CO2 hydrogenation is still under debate. This paper describes an experimental study on the nature of surface-bound hydroxyl groups over Al2O3-supported Cu catalysts for CO2 reduction. A model 5 wt % Cu/Al2O3 catalyst with stable hydroxyl groups was prepared. The structural hydroxyl groups were modulated by the hydration of unsaturated Al3+ sites, which were introduced by the evaporation-induced self-assembly method. Terminal hydroxyl groups (T-OH*) were found to significantly facilitate the conversion of CO2, while the AlVI-T-OH and AlIV-T-OH species promoted the formation of Al-b-HCOO and Al-m-HCOO species, respectively, accompanied with the increase in methanol and dimethyl ether yields. The reaction behavior of hydroxyl species was further investigated by in situ IR experiments with HD isotope exchange on Cu/Al2O3. T-OH* were identified as active sites participating in the formation of key intermediates, while more hydroxyl sites were occupied by formate species with the H coadsorbed on the Cu surfaces.
研究领域:
催化
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化学工程
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表面科学
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产品关联
DOI
高影响因子
Journal of Physical Chemistry C
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2024
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IF 3.3
Cong Fu,Lingfang Liu,Cici Wang,Weixin Huang,Guofeng Zhao
Unraveling the effect of defects on the concentration of surface-available photoexcited charges is of great importance for semiconductors in photocatalysis. Herein, by using in situ diffuse-reflectance infrared (IR) spectroscopy, the concentration of surface-available photoholes on TiO2 nanoparticles with tunable bulk/surface defects was quantified by an adsorbate (methanol) surface elementary reaction kinetic analysis method. Reaction kinetics showed that the oxidation of the adsorbed methanol species under light irradiation was a first-order reaction. Therefore, the concentration of surface-available photoholes can be calculated from the rate constants of adsorbed methanol on the TiO2 surface. By carefully comparing the specific reaction rate constants on the TiO2 surface with various bulk/surface defect ratios, we demonstrated for the first time that increasing the bulk defect concentration relative to the surface defects decreases the concentration of surface-available photoholes. This trend implicates different effects of bulk and surface defects on band bending and subsequent interfacial hole transfer processes in TiO2 nanoparticles. These insights not only reveal the mechanistic role of surface and bulk defects in photocatalysis but also highlight that in situ IR spectroscopy combined with reaction kinetic analysis has enormous potential in elucidating photocatalytic mechanisms.
研究领域:
光催化
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材料化学
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表面科学
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物理化学
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纳米材料
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分析化学
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DOI
高影响因子
JOURNAL OF PHYSICAL CHEMISTRY A
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2020
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IF 2.6
Tao Wang,Yangyang Liu,Yue Deng,Hanyun Cheng,Xiaozhong Fang,Liwu Zhang
The heterogeneous reaction of SO2 on manganese oxides is poorly understood. By means of in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), this study investigated the reaction kinetics and product fractions on four types of manganese oxides. Due to the positive and negative moisture impacts, 68% RH (relative humidity) becomes the most favorable condition for the uptake of SO2. Mn3O4 shows the greatest uptake capacity of SO2, followed by MnO2 and Mn2O3, with that of MnO being the weakest. Curve-fitting procedures were undertaken to further dissect the product spectra. Increased RH facilitates the physical adsorption of SO2 and generally weakens the oxidation capacity of manganese oxides. The oxidation ability is greatest for MnO, followed by MnO2 and Mn3O4, with that of Mn2O3 being the weakest. Additionally, the particle acidity (pH) was estimated by the ionization equilibrium of sulfurous acid and the relative contributions of S(IV) species. MnO and Mn3O4 become more acidic as RH increases while Mn2O3 and MnO2 are the most acidic at 50% RH, which can be attributed to the different uptake capacities of SO2 and H2O on each sample. Overall, for the heterogeneous reaction of SO2 on manganese oxides, both particle type and moisture condition influence the reaction kinetics and product fractions. This work improves the understanding of the heterogeneous process on atmospheric manganese-rich particles.
研究领域:
环境化学
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大气科学
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表面化学
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气溶胶化学
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物理化学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Shuhan Lu,Jiao He,He Jiang,Yixiao Wang,Ruirui Hu,Xiang Gong,Bin Wang,Chunhai Yi,Fusheng Yang,Tao Fang
The liquid organic hydrogen carrier (LOHC) technology distinguishes itself among various hydrogen storage technologies owing to its distinctive advantages. However, conventional hydrogenation reaction processes generally necessitate elevated hydrogen pressure (5–8 MPa). This study presents an electrocatalytic hydrogenation reaction (ECH) system utilizing N -methylindole (NMID) as the substrate. The system not only achieves hydrogenation reactions using water as the hydrogen source under ambient pressure, but also attains a selectivity exceeding 70 % for the fully hydrogenated product (8H-NMID) via the synergistic catalytic effects of Pt and Ru. Furthermore, the hydrogenation pathway of NMID was elucidated through in-situ infrared spectroscopy and Gaussian theoretical calculations. This research establishes the feasibility of LOHC hydrogenation through ECH, providing innovative perspectives for LOHC technology applications.
研究领域:
物理化学
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催化化学
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能源材料
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电化学
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氢储能技术
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产品关联
DOI
高影响因子
JOURNAL OF CATALYSIS
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2018
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IF 6.759
Xiaolong Liu,Qingzhen Han,Wenbo Shi,Cheng Zhang,Erwei Li,Tingyu Zhu
In this work, ruthenium-based bimetallic catalysts of 1Ru-5 M/TiO 2 (M = Co, Ce, Fe, Mn, Cu, Ni) were prepared and evaluated in ethyl acetate oxidation. It was found that 1Ru-5Cu/TiO 2 gave the highest catalytic activity. The influence of CuO content and the preparation method on the catalytic activity was also studied. 1Ru-5Cu/TiO 2 showed great catalytic stability in the on-stream reaction test. The influence of H 2 O on the catalytic activity is presented. The bimetallic catalyst 1Ru-5Cu/TiO 2 showed better catalytic performance than the monometallic catalysts 1Ru/TiO 2 and 5Cu/TiO 2 . XRD, TEM, HAADF-STEM, H 2 -TPR, and XPS characterizations were conducted, and the synergistic effect between Ru and Cu was well presented. In situ FTIR studies were also conducted, and the reaction intermediates were revealed on the catalyst surface. The theoretical calculations suggested that ethyl acetate is more easily adsorbed on the CuO surface, while it reacts more easily on the RuO 2 surface . Accordingly, a reaction mechanism for the catalytic oxidation of ethyl acetate over a Ru-Cu bimetallic catalyst is proposed.
研究领域:
催化化学
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环境化学
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表面科学
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材料化学
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物理化学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）