Molecular Catalysis
·
2025
·
IF 4.9
Hui Kang,Quan Shao,Luming Li,Yanlin Zhang,Xin Xiao,Yuefeng Liu
The gas-inducing strategy has proven highly effective in constructing high-density oxide interfaces. In this study, we utilized CO 2 hydrogenation reaction to induce the spontaneous dispersion of In 2 O 3 species on the surface of TiO 2 , forming numerous InO x /TiO 2 interfaces. The 2 %In 2 O 3 /TiO 2 catalyst demonstrated a 33-fold enhancement in reverse water-gas shift reaction (RWGS) performance after dispersion. Multi-technique characterization revealed that H 2 in the reactants reduced In 2 O 3 to partially reduced states (In +(3-x) ), which were more prone to migration. The spontaneous dispersion was not solely driven by the strong interaction (anchoring) ability of the support for In 2 O 3 species. Further mechanistic studies showed that the high-density InO x /TiO 2 interface formed via spontaneous dispersion significantly promoted the formation of formate species during CO 2 hydrogenation, which decomposed into CO at lower temperatures (297 °C), thereby improving catalytic performance. This work highlights the potential of atmosphere-induced structural evolution in catalysis, underscoring the importance of a comprehensive analysis of the activation, migration, and anchoring mechanisms, as well as the catalytic promotion principles of the induced structure.
研究领域:
催化化学
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材料科学
·
表面科学
✓ 已验证
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2020
·
IF 6.182
Yudong Zhang,Long Liang,Ziyang Chen,Jinjun Wen,Wen Zhong,Sibei Zou,Mingli Fu,Limin Chen,Daiqi Ye
Self-assembled CeO 2 with 3D hollow nanosphere, nanoparticle and nanocube morphologies were prepared and used to support Cu particles. The obtained samples (denoted as Cu/CeO 2 -hs, Cu/CeO 2 -np and Cu/CeO 2 -nc, respectively) were tested for the reverse water-gas shift (RWGS) reaction. Under the reaction conditions, V (H 2 ): V (CO 2 ) = 3:1 and weight hourly space velocity (WHSV) = 300,000 mL g −1 h −1 , the Cu/CeO 2 -hs sample exhibited the best catalytic performance among the as-prepared catalysts. In order to reveal the key factors affecting the catalytic performance, the physicochemical properties of the catalysts were analyzed by XRD, BET, SEM, TEM, H 2 -TPR, quasi in-situ XPS and in situ UV-Raman techniques. The results point out that the particle size of Cu is not the rate-determining factor while the amount of surface oxygen vacancies is highly correlated with the catalytic reaction rate. In situ UV-Raman and in situ DRIFTS experiments indicate the formation of bidentate carbonate and formate species on oxygen vacancy sites which is thought to be the key intermediates for the RWGS reaction. These findings unravel the crucial roles of surface oxygen vacancies on CO 2 adsorption and activation and also highlight a feasible way for the design of highly efficient catalysts for the important RWGS reaction in chemical industry.
研究领域:
催化化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Qiufeng Liu,Kaihang Sun,Kun Lu,Xingwei Xie,Longzhou Zhang,Young Dok Kim,Zhongyi Liu,Zhikun Peng
Metal-support interaction (MSI) is an efficient strategy to modulate the distribution of active metal with different electronic states over the oxide-supported metal catalysts. However, the intrinsic correlation between the intensity of MSI and the electronic structure of supported metals remains inadequate. In this work, the intensity of MSI over the Cu/Y 2 O 3 catalyst was tuned by the calcination temperature, which regulated the distribution of Cu 0 , Cu + and Cu 2+ species. The Cu/Y 2 O 3 catalyst with the highest amount of Cu + exhibits the superior performance of reverse water–gas shift reaction. Due to the enhanced H 2 activation and promoted charge transfer at the interfacial Cu + /Y 2 O 3 site based on the experimental characterizations, the CO formation rate reached 220 mmol CO g cat −1 h −1 at 500 °C. The present work provides an efficient way to regulate the supported metal species with the specific electronic state.
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JACS Au
·
2025
·
IF 8.7
Xuan Bie,Yukun Pan,Xiaowei Wang,Shiyu Zhang,Jiahui Hu,Xiaoxiao Yang,Qinghai Li,Yanguo Zhang,Robert E. Przekop,Yayun Zhang,Hui Zhou
Gas sources rich in CO2 derived from biomass/waste gasification, anaerobic digestion, or industrial carbon capture often contain impurities such as H2S, H2O, and NH3, which can significantly hinder catalyst performance. Here, we show the role of NH3 on the reverse water–gas shift (RWGS) reaction over a commercial Cu/ZnO/Al2O3 catalyst, examining its effects on both the catalytic activity and the catalyst structure. We found that NH3 reversibly decreases CO2 conversion immediately by suppressing carbonate hydrogenation and CO desorption. This effect intensifies with an increase in NH3 concentration but decreases at higher temperatures. However, prolonged exposure (over 100 h) to RWGS conditions in the presence of 1.4% NH3 leads to near-total and irreversible deactivation of the Cu/ZnO/Al2O3 catalyst. Under NH3 exposure, the catalyst loses Cu+ sites on the surface, causing a spatial separation of Cu and ZnO. Finally, to address this challenge, we propose a novel strategy to mitigate NH3 inhibition by decomposing NH3 into N2 and H2.
研究领域:
化学工程
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催化科学
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环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Catalysis Science & Technology
·
2020
·Vol. 10
·期 8
·2343-2352
·
IF 5.721
Ziheng Zhen,Wenxiang Tang,Wei (Willy) Chu,Tao Zhang,Li Lv,Shengwei Tang
The dispersity and the neighboring degree of different sites play crucial roles in the catalytic performance of dual site catalysts. The solution of precursors was encapsulated into microdroplets by forming a microemulsion. The average diameter of microdroplets was about 45 nm. This guaranteed that the dosage of precursors was at the attogram level and only about a thousand precursor molecules were encapsulated in each microdroplet. An anti-solvent extraction method was applied to extract water from the microdroplets with acetonitrile. The precursors co-precipitated in the microdroplets due to the loss of water. The encapsulated precursors in the microdroplets co-precipitated together in nanoscale space, so the neighboring degree of the two precursors was improved significantly. The prepared catalyst was characterized by ICP-OES, BET, XRD, H2-TPR, TEM and XPS. Compared with the Cu–ZnO/Al2O3 (CZA) catalysts prepared by the conventional impregnation method, the CZA catalysts prepared by the proposed strategy had much stronger interaction and a better neighboring degree of the dual active sites. They also showed very good catalytic performance for the reverse water gas shift (RWGS) reaction. The CO2 conversion of the designed CZA catalysts was about 1–2 times higher than that of the CZA catalysts prepared by the conventional impregnation method at 0.1 MPa, 300–400 °C and a CO2/H2 mole ratio of 1.
研究领域:
催化化学
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材料科学
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环境工程
✓ 已验证
产品关联
DOI
高影响因子
GREEN CHEMISTRY
·
2025
·
IF 9.2
Chenfei Yao,Boyu Zhu,Peng Zheng,Xingbang Hu
A catalytic system containing (Ru(CO)3Cl2)2, LiCl, ionic liquid and organic base was reported, which could effectively promote the following processes: low-temperature reverse water gas shift (RWGS) (at 100 oC), hydroformylation and hydrogenation of butyraldehyde to butanol, enabling the direct synthesis of butanol from propylene and CO2. The possible catalytic mechanism and the role of each additive were proposed based on the detection of reactive intermediates, control experiments and theoretic calculations. The critical step in this transformation is achieving RWGS at low temperatures without external reductants or dehydrating agents. Up to 99% conversion of propylene with 97% selectivity of butanol (n:i=1.4) was achieved, which represents the highest yield to date. Meanwhile, the catalytic system could maintain a certain degree of stability during recovery process. The results reported here may create a chance for the industrial application of the direct synthesis of butanol from propylene and CO2.
研究领域:
化学工程
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
RSC Advances
·
2025
·Vol. 15
·期 11
·8346-8353
·
IF 4.6
Qingshan Rong,Wei Ding,Guogang Liu,Xiangyu Fu,Yan Shi,Zhiqiang Zhang,Zhiwei Yao
In this study, we found that β-Mo2C prepared at different carbonization temperatures exhibited significantly different catalytic activities for the reverse water gas shift (RWGS) reaction. The β-Mo2C synthesized at 600 °C demonstrated notably higher activity compared to those prepared at 700 °C and 800 °C. This enhanced activity was likely attributed to its improved redox properties, which were primarily driven by a smaller crystallite size and the presence of MoxOCy species. Therefore, we proposed that the crystallite size and MoxOCy content were the key factors governing the RWGS activity of β-Mo2C. Clearly, both factors were strongly influenced by the carbonization temperature. Notably, the β-Mo2C prepared at 600 °C even outperformed Cu-doped β-Mo2C prepared at 700 °C under similar reaction conditions.
研究领域:
催化化学
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Bowen Lu,Tai Zhang,Liqi Zhang,Yongqing Xu,Zewu Zhang,Fan Wu,Xiaoshan Li,Cong Luo
CeO 2 -based catalysts have been widely used in the CO 2 hydrogenation process. The oxygen vacancies on CeO 2 resulted from Na ion incorporation play a vital role in CO 2 conversion activity, the effect of Na + ion-doped in CeO 2 during CO 2 hydrogenation was rarely studied. In this work, the LN-CeO 2 catalysts with different n NaOH :n Ce ratios were prepared with liquid nitrogen(Liquid Nitrogen-CeO 2 , LN-CeO 2 ), and the effect of the n NaOH :n Ce ratio on the microstructure of the LN-CeO 2 catalysts were evaluated. The best CO 2 hydrogenation performance was achieved by LN-CeO 2 -100 with a CO production rate of 3.90 mol/g cat· h at 800 °C (100% CO selectivity). The kinetic results indicated that the CO 2 hydrogenation performance difference among these LN-CeO 2 catalysts resulted from the CO 2 activation process. Oxygen vacancies could enhance CO 2 activation on the surface of LN-CeO 2 , and oxygen vacancies displayed a linear correlation relationship with the Na content doped in LN-CeO 2 . The highest concentration of oxygen vacancies resulted from Na ion incorporated and lower CO 2 reaction order was closely related to CO 2 hydrogenation performance of LN-CeO 2 -100. These results will give insight into the Na effect on the CO 2 hydrogenation mechanism over CeO 2 .
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Jie Chu,Jialin Guo,Yafei Guo,Benshuai Guo,Pu Huang,Zhouzhou Zhang,Chuanwen Zhao
Integrating CO 2 capture and utilization (ICCU) in the production of syngas for the C1 chemical industry through ICCU-RWGS (reverse water–gas shift reaction) is a vital strategy for achieving carbon reduction, and designing highly active dual-functional materials (DFMs) capable of CO 2 adsorption and in-situ conversion is crucial. Alkaline lithium ceramics with high availability, featuring high CO 2 capture and catalytic performance, are promising DFMs candidates for ICCU-RWGS. Herein, lithium ceramics of Li 5 FeO 4, Li 6 CoO 4 and Li 6 ZnO 4 were prepared via solid state synthesis as potential DFMs for ICCU-RWGS applications, and structure-property-activity relationships of the lithium ceramics DFMs in ICCU were discussed. The Li-Zn sample with high surface basicity and high density and uniform dispersion of active sites demonstrated a high CO 2 uptake (7.71 mmol CO 2 /g), CO yield (6.52 mmol CO/g), CO 2 conversion (84.9 %) and CO selectivity (∼100 %) as well as moderate CO 2 adsorption and hydrogenation kinetics at 650 °C, 10 %CO 2 and 40 %H 2 , making it a promising candidate for ICCU-RWGS. However, the Li-Zn DFMs exhibited poor cyclic ICCU-RWGS working stability due to lithium sublimation and crystal sintering at high temperatures, which deserves more future efforts to solve the dilemma. Our findings provide valuable insights into designing cost-effective DFMs for ICCU applications.
研究领域:
化学工程
·
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2024
·
IF 4.1
Qiangqiang Wu,Hongquan Fu,Chengxiong Dang,Guangxing Yang,Yonghai Cao,Hongjuan Wang,Hao-Fan Wang,Hao Yu
The reverse water–gas shift (RWGS) reaction has been identified as one of the most techno-economically viable strategies for handling with antropogenic CO 2 emissions, but high-efficiency RWGS catalysts are still challenging. Herein, a series of In-modified Ni-based catalysts with variations of the support and the Ni/In ratio were prepared by a simple wet impregnation method. The high activity for RWGS reaction is achieved on the CeO 2 -supported catalysts. The incorporation of In into Ni/CeO 2 catalysts significantly increases CO selectivity. The optimal 10Ni-5In-CeO 2 catalyst shows 97.2 % CO selectivity at CO 2 conversion rate of 52.8 mmol g Ni −1 h −1 for 100 h without obvious deactivation at 350 °C. The oxygen vacancies on CeO 2 and the active *H species on Ni-In intermetallic compounds (IMCs) are responsible for the enhancement of RWGS reaction. This work provides a guidance to high-efficiency catalysts for CO 2 hydrogenation by cooperation between active metal and oxide support.
研究领域:
催化化学
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材料科学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Catalysis
·
2021
·
IF 13.084
Mengwei Gu,Sheng Dai,Runfa Qiu,Michael E. Ford,Chenxi Cao,Israel E. Wachs,Minghui Zhu
The reverse water–gas shift (RWGS) reaction is an initial and essential step for CO2 hydrogenation. In this study, Cu- and K-modified iron oxide catalysts were investigated with a series of in/ex-situ characterization techniques, including in situ XRD, in situ Raman, in situ DRIFTS quasi in situ XPS, quasi in situ HS-LEIS, H2-TPR, CO2-TPD, and TPSR. The surface structure of the catalyst is found to strongly depend on the presence of Cu and K, leading to diverse reducibility and basicity. Adding K to the iron-based catalyst alters the reaction from a redox pathway that proceeds on surface redox sites to an associative pathway that proceeds on surface redox and basic sites. Metallic Cu facilitates hydrogen dissociation and promotes both mechanisms by either boosting surface vacancy sites or supplying abundant surface hydrogen atoms. These findings would be beneficial for the rational design of CO2 hydrogenation catalysts.
研究领域:
催化化学
·
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
Carbon Capture Science & Technology
·
2023
·
IF 0
Bowen Lu,Fan Wu,Xiaoshan Li,Cong Luo,Liqi Zhang
The interfacial structure of metal and oxide support plays a pivotal role in reverse water gas shift (RWGS). However, rare work investigated the factor of the metal-oxide interface during RWGS reaction. In this work, the interface of Cu/CeO 2 catalysts was designed through the thermal treatment of copper nitrate salt on CeO 2 with an H 2 atmosphere under different temperatures, and CO 2 hydrogenation performance was studied at 400 °C to investigate the effect of interfacial structure on RWGS reaction. Among these prepared catalysts, Cu/CeO 2 -400 catalysts achieved the best CO 2 conversion activity (CO production rate 1.23 mol/g cat . h). Cu interacted with CeO 2 to form Cu-O-Ce interface and induced more oxygen vacancy formation. The oxygen vacancy around the Cu-CeO 2 interface enhanced CO 2 adsorption and promoted CO 2 conversion. CO 2 reacted with active hydrogen to COOH, then COOH species dissociated into CO and OH adsorbed on the surface of Cu-CeO 2 . These results gave insights into the design of a highly effective catalyst for CO 2 hydrogenation.
研究领域:
催化化学
·
材料科学
·
能源化学
✓ 已验证
DOI
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