JOURNAL OF CATALYSIS
·
2024
·
IF 6.5
Peng Zhang,Fangfang Li,Xuefang Yao,Pengze Zhang,Yukai Wu,Mengmeng Xi,Fanhui Meng,Lihua Kang,Mingyuan Zhu
The GaZrO x solid solution has been recently employed in OX-ZEO bifunctional catalysts for efficient conversion of syngas to light olefins, but it remains challenging to identify the specific contributions of Zr and Ga and to understand the detailed reaction mechanisms due to the structural complexity. To address this complexity and elucidate the active sites over the Zr-Ga oxide system, this study presents a catalyst designed by physical mixing ZrO 2 with different crystalline phases ( m -ZrO 2 & t -ZrO 2 ) and α -Ga 2 O 3 . The physical mixture of m -ZrO 2 and α -Ga 2 O 3 achieves a high CO conversion of 39.1 %, with light olefins selectivity of 87.3% among hydrocarbons after combined with SAPO-34, surpassing the performance of physical mixture of t -ZrO 2 and/or α -Ga 2 O 3 with SAPO-34. Combining the various characterizations and DFT calculations, we have confirmed that m -ZrO 2 site, enriched with oxygen vacancies and surface hydroxyl groups, is essential for CO adsorption and HCOO* intermediate formation, while the α -Ga 2 O 3 site plays a key role in the dissociation of H 2 . Furthermore, the electron transfer from m -ZrO 2 to α -Ga 2 O 3 in their mixture is more efficient than in a physically mixed t -ZrO 2 and α -Ga 2 O 3 . This accelerates the H 2 dissociation and boosts the spillover of hydrogen from α -Ga 2 O 3 to m -ZrO 2 , leading to the formation of more CH 3 O* intermediates and higher light olefins yield when combined with SAPO-34.
研究领域:
催化化学
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材料科学
·
计算化学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
·
2021
·
IF 5.706
Min Zhao,Yihui Li,Ziang Zhao,Yuan Lyu,Wei Lu,Hejun Zhu,Yunjie Ding
Mn-doped spinel oxides CoAl 2 O 4 marked as CMA-m (m = Co/Mn atom ratio) herein were synthesized and evaluated for the first time as supports of Co-based Fischer-Tropsch synthesis (FTS) catalysts. HAADF-STEM images showed that Mn doping caused more crystal defects on the surface of CMA-m grains, which may provide more attachment sites for cobalt loading, leading to much smaller Co 0 particle size of 15Co/CMA-m than that of 15Co/CoAl 2 O 4 . Data of H 2 /CO chemisorption showed that the interaction of highly dispersed Co 0 with lattice Mn-doped CMA-m grain has a promotive effect on CO adsorption capability. FTS evaluation results demonstrate that 15Co/CMA-20 showed the highest CO conversion, C 5+ selectivity and C 5+ STY, benefiting from its high Co 0 dispersion and CO chemisorption capability as a result of suitable Mn doping into the lattice of CoAl 2 O 4 , which was confirmed very different from the influence of impregnated Mn oxide over CoAl 2 O 4 .
研究领域:
催化化学
·
材料科学
✓ 已验证
DOI
高影响因子
JOURNAL OF CATALYSIS
·
2020
·
IF 7.888
Jichang Lu,Jian Fang,Zhizhi Xu,Dedong He,Siyou Feng,Yubei Li,Gengping Wan,Sufang He,Hua Wu,Yongming Luo
Supported MoS 2 based materials are widely used as heterogeneous catalysts. In this work, we propose a rapid and facile method (ultrasound-induced impregnation assisted by microwave thermal treatment) to synthesize mesoporous silica (SBA-15)-supported, few-layer, ordered and K-promoted MoS 2 nanosheets with different K/Mo ratios. The prepared catalysts are characterized by various physical and chemical techniques. Their catalytic performance is evaluated by methyl mercaptan (CH 3 SH) synthesis from CO/H 2 /H 2 S. The results show that our catalysts exhibit a much higher CO conversion and selectivity to CH 3 SH than the catalysts prepared using the conventional impregnation and reported in the literature. The good performance arises because of two main factors: MoS 2 nanosheets of only 2–4 layers and K promotion. Experimental characterizations and (density functional theory) calculations show that the former is the typical nano-size effect, and the latter stabilizes C S bonds when activating COS molecules.
研究领域:
催化材料
·
物理化学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Jiaxin Li,Yifei Liang,Zhao Li,Ke Fan,Chunxue Wang,Kai Li,Yuan Li,Xin Sun,Ping Ning,Fei Wang
The synthesis of methane from syngas represents a pivotal technology in the artificial synthesis of natural gas, with the study of methanation catalysts being a fundamental aspect of this process. Extensive research has focused on CO methanation using Ni/Al 2 O 3 catalysts; however, enhancements in catalyst stability and low-temperature activity are still required. This research investigated the structure of Ni/Al 2 O 3 under H 2 reduction at varying temperatures and the catalytic performance in natural gas synthesis (SNG) through CO methanation. It was observed that a higher reduction temperature resulted in nickel species agglomeration. Notably, Ni catalysts reduced at 600 °C demonstrated optimal CO conversion and CH 4 selectivity under the tested conditions. Characterization studies uncovered a synergistic effect between Ni and NiO species, which was most effective for catalytic activity under hydrogen reduction at 600 °C but only at an appropriate reduction temperature. These insights are significant for the advancement of Ni/Al 2 O 3 methanation catalysts in natural gas production .
研究领域:
化学工程
·
催化科学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED ORGANOMETALLIC CHEMISTRY
·
2019
·Vol. 33
·期 11
·e5208
·
IF 3.259
Baowei Wang,Chengyu Wang,Wenxian Yu
Mo 2 C/Al 2 O 3 catalyst was prepared by the impregnation method with urotropine and ammonium paramolybdate. The catalytic effect of Mo 2 C as a typical transition-metal carbide in sulfur-resistant methanation was studied. The catalysts prepared were characterized by N 2 adsorption–desorption, X-ray diffraction, transmission electron microscopy, H 2 -temperature-programmed reduction, and Raman spectra, with the results confirming the formation of β-molybdenum carbide on the surface of the catalysts. Studies on catalysts with different loading doses indicate that the optimal loading of Mo 2 C/Al 2 O 3 is about 15 wt.%, which enables CO conversion rate of up to 47%, with methane selectivity of up to 53%. This work further explored the effect of different concentrations of H 2 S in the raw gas on the performance of the catalyst, with the results showing that high concentration of H 2 S (>1500 ppm) can lead to sulfuration of active species on the catalyst, while resulting in a decrease in the catalytic activity.
研究领域:
催化化学
·
材料科学
✓ 已验证
DOI
高影响因子
JOURNAL OF THE ENERGY INSTITUTE
·
2020
·
IF 4.748
Min Wang,Shupeng Guo,Ming Xia,Jungang Wang,Zhongyi Ma,Bo Hou,Litao Jia,Debao Li
Whether Co-ZrO 2 interfacial sites have a beneficial effect on Co-based Fischer-Tropsch synthesis is still controversial. In this paper, different quantities of Co-ZrO 2 interfacial sites were fabricated by changing the impregnation sequence of Zr added to Co/SiC catalysts. The effect of the Co-ZrO 2 interfacial sites was investigated by nitrogen adsorption, X-ray diffraction (XRD), hydrogen chemisorption (H 2 -TPD), temperature-programmed reduction (H 2 -TPR) and TEM-EDS- mapping analyses. It was found that when zirconium was on the surface of cobalt, more Co-ZrO 2 interfacial sites were formed, and a higher selectivity of long-chain hydrocarbons was observed. In addition, the formation of Co-ZrO 2 interfacial sites significantly increased the conversion frequency of CO. This work is of great significance for understanding the role of Co-ZrO 2 interfacial sites and guiding the design of related catalysts in Co-based Fischer-Tropsch synthesis.
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
Nature Communications
·
2024
·Vol. 15
·期 1
·1-11
·
IF 14.7
Xue Jing,Dong Xue,Liu Chunxiao,Li Jiawei,Dai Yizhou,Xue Weiqing,Luo Laihao,Ji Yuan,Zhang Xiao,Li Xu,Jiang Qiu,Zheng Tingting,Xiao Jianping,Xia Chuan
Using renewable electricity to convert CO 2 into CO offers a sustainable route to produce a versatile intermediate to synthesize various chemicals and fuels. For economic CO 2 -to-CO conversion at scale, however, there exists a trade-off between selectivity and activity, necessitating the delicate design of efficient catalysts to hit the sweet spot. We demonstrate here that copper co-alloyed with isolated antimony and palladium atoms can efficiently activate and convert CO 2 molecules into CO. This trimetallic single-atom alloy catalyst (Cu 92 Sb 5 Pd 3 ) achieves an outstanding CO selectivity of 100% (±1.5%) at −402 mA cm −2 and a high activity up to −1 A cm −2 in a neutral electrolyte, surpassing numerous state-of-the-art noble metal catalysts. Moreover, it exhibits long-term stability over 528 h at −100 mA cm −2 with an FE CO above 95%. Operando spectroscopy and theoretical simulation provide explicit evidence for the charge redistribution between Sb/Pd additions and Cu base, demonstrating that Sb and Pd single atoms synergistically shift the electronic structure of Cu for CO production and suppress hydrogen evolution. Additionally, the collaborative interactions enhance the overall stability of the catalyst. These results showcase that Sb/Pd-doped Cu can steadily carry out efficient CO 2 electrolysis under mild conditions, challenging the monopoly of noble metals in large-scale CO 2 -to-CO conversion.
研究领域:
材料科学
·
化学工程
·
电化学
·
可持续能源
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CERAMICS INTERNATIONAL
·
2025
·
IF 5.6
Liqing Chen,Kejia Fan,Luting Yan,Jingfa Yang
Global economic and technological advancements have led to a significant surge in CO 2 emissions, posing severe environmental challenges. This study explores the photocatalytic reduction of CO 2 using a high-entropy fluorite oxide (HEFO), (Ce 0.2 Zr 0.2 Ti 0.2 Sn 0.2 Ca 0.2 )O 2-δ , synthesized via solid-state reactions. XRD, SEM, and XPS analyses confirmed a single-phase fluorite structure and revealed excellent light absorption (250–400 nm) with a 2.6 eV bandgap. Photocatalytic CO 2 reduction experiments demonstrated the superior performance of fine particles (72 % CO 2 conversion, 12.01 μmol h −1 g −1 methane generation, 61.2 % selectivity) compared to that of coarse one. This enhanced activity was attributed to a higher oxygen vacancy concentration, which optimized the surface electronic structure, increased the number of active sites, and improved CO 2 adsorption and activation. This study highlights the potential of HEFOs for renewable fuel production via CO 2 photoreduction.
研究领域:
环境科学
·
材料化学
·
催化
·
可再生能源
✓ 已验证
产品关联
DOI
高影响因子
Catalysis Science & Technology
·
2022
·Vol. 12
·期 14
·4624-4636
·
IF 6.177
Yi Yang,Weixin Qian,Haitao Zhang,Zhonghao Han,Hongfang Ma,Qiwen Sun,Weiyong Ying
FeMnxZr and FeMnxZr2Na catalysts prepared by coprecipitation and impregnation methods were applied to investigate the promoting effects of Zr on iron-based catalysts for high-temperature Fischer–Tropsch synthesis (HTFT). Ar physisorption and TEM demonstrated that Zr-promoted catalysts have a larger BET surface area and larger pore volume, which are more conducive to the distribution of active phases. Zr promoted the dispersity of iron particles and reduced the grain size of iron particles, resulting in the improvement of the FTS activity. The CO-TPD and MES results revealed that the introduction of Zr promoted the dissociative adsorption of CO, thereby promoting the formation of the active phase χ-Fe5C2 while suppressing the formation of ε′-Fe2.2C and further improving the FTS activity and the selectivity to C2=–C4= in the hydrocarbon distribution. However, the addition of an excessive amount of Zr caused the excess ZrO2 to cover the surface of the active site, inhibiting the CO dissociative adsorption and the formation of χ-Fe5C2, resulting in a decrease in the CO conversion and the selectivity to C2=–C4=. The XPS and H2-TPR results proved the interaction between Fe2O3 and ZrO2. And the Fe–ZrO2 interaction inhibited the coke deposition and aggregation of the Fe species, as confirmed by XRD and TEM, respectively. The FeMn5Zr2Na catalyst exhibited the highest C2=–C4= selectivity of 34.4% at a CO conversion of 96.3%. And FeMn5Zr2Na displayed the highest production of light olefins (441.6 g h−1 kgCat−1), which was significantly higher than FeMn2Na (162.2 g h−1 kgCat−1).
研究领域:
催化
·
化学工程
·
材料科学
✓ 已验证
DOI
高影响因子
JOURNAL OF THE ENERGY INSTITUTE
·
2024
·
IF 5.6
Haonan Zheng,Yiran Zhang,Zibo Xu,Guangzhao Zhou,Xuteng Zhao,Zhen Huang,He Lin
High entropy oxides (HEOs) show great prospects in catalysis owing to their widely tunable component structures and ease of combination with active metals. However, the development of HEO catalysts is limited by the lack of efficient synthesis methods due to the difficulty of homogeneously mixing at least five elements. In this work, flame spray pyrolysis (FSP) is successfully employed to synthesize (CrMnFeCoNi) 3 O 4 HEO with a single phase spinel structure in one step, which is verified by X-ray diffraction (XRD), high-resolution transmission electron microscopy (HRTEM), selected area electron diffraction (SAED), and energy-dispersive X-ray spectroscopy (EDS). Taking CO catalytic oxidation as a probe reaction, the Pt@(CrMnFeCoNi) 3 O 4 HEO catalyst synthesized by FSP in one step is compared with the catalyst whose Pt is impregnated on (CrMnFeCoNi) 3 O 4 HEO support. The FSP-made catalysts have a higher catalytic reaction rate and better redox ability, which lowers the temperature of complete CO conversion by nearly 100 °C. Furthermore, it can be observed that the flame parameters can be optimized to modify the particle size and oxygen vacancies of the HEO nanoparticles, thus enhancing the catalytic performances. This work demonstrates that FSP is an effective method for the one-step synthesis of HEO catalysts with excellent catalytic performance, providing a new perspective for the synthesis of HEO-based materials.
研究领域:
材料科学
·
催化
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-11
·
IF 14.7
Li Hefei,Wei Pengfei,Liu Tianfu,Li Mingrun,Wang Chao,Li Rongtan,Ye Jinyu,Zhou Zhi-You,Sun Shi-Gang,Fu Qiang,Gao Dunfeng,Wang Guoxiong,Bao Xinhe
Producing valuable chemicals like ethylene via catalytic carbon monoxide conversion is an important nonpetroleum route. Here we demonstrate an electrochemical route for highly efficient synthesis of multicarbon (C 2+ ) chemicals from CO. We achieve a C 2+ partial current density as high as 4.35 ± 0.07 A cm −2 at a low cell voltage of 2.78 ± 0.01 V over a grain boundary-rich Cu nanoparticle catalyst in an alkaline membrane electrode assembly (MEA) electrolyzer, with a C 2+ Faradaic efficiency of 87 ± 1% and a CO conversion of 85 ± 3%. Operando Raman spectroscopy and density functional theory calculations reveal that the grain boundaries of Cu nanoparticles facilitate CO adsorption and C − C coupling, thus rationalizing a qualitative trend between C 2+ production and grain boundary density. A scale-up demonstration using an electrolyzer stack with five 100 cm 2 MEAs achieves high C 2+ and ethylene formation rates of 118.9 mmol min −1 and 1.2 L min −1 , respectively, at a total current of 400 A (4 A cm −2 ) with a C 2+ Faradaic efficiency of 64%.
研究领域:
电化学
·
催化
·
材料科学
·
能量转换
✓ 已验证
DOI
PubMed
高影响因子
CHEMISTRY-A EUROPEAN JOURNAL
·
2018
·Vol. 24
·期 34
·8596-8602
·
IF 5.16
Yong Xu,Jiang Mo,Zi-Cheng Fu,Su Liu,Zhi Yang,Wen-Fu Fu
Graphical A hybrid photocatalyst consisting of Co and Co 2 P nanoparticles embedded in N, P-codoped carbon nanosheets was used in a visible light-driven system for CO 2 -to-CO conversion. The catalytic system displayed a high CO production rate of up to 35 000 μmol h −1 g −1 with CO selectivity of 79.1 % in the first 3 h of reaction. Linear CO production at an exceptionally high rate of 63 000 μmol h −1 g −1 was observed in the first 1 h of photocatalytic reaction. Artificial photosynthesis has attracted wide attention, particularly the development of efficient solar light-driven methods to reduce CO 2 to form energy-rich carbon-based products. Because CO 2 reduction is an uphill process with a large energy barrier, suitable catalysts are necessary to achieve this transformation. In addition, CO 2 adsorption on a catalyst and proton transfer to CO 2 are two important factors for the conversion reaction, and catalysts with high surface area and more active sites are required to improve the efficiency of CO 2 reduction. Here, a visible light-driven system for CO 2 -to-CO conversion is reported, which consists of a heterogeneous hybrid catalyst of Co and Co 2 P nanoparticles embedded in carbon nanolayers codoped with N and P (Co-Co 2 P@NPC) and a homogeneous Ru II -based complex photosensitizer. The average generation rate of CO of the system was up to 35 000 μmol h −1 g −1 with selectivity of 79.1 % in 3 h. Linear CO production at an exceptionally high rate of 63 000 μmol h −1 g −1 was observed in the first hour of reaction. Inspired by this highly active catalyst, Co@NC and Co 2 P@NPC materials were also synthesized and their structure, morphology, and catalytic properties for CO 2 photoreduction were explored. The results showed that the nanoparticle size, partially adsorbed H 2 O molecules on the catalyst surface, and the hybrid nature of the systems influenced their photocatalytic CO 2 reduction performance.
研究领域:
材料科学
·
催化
·
光化学
·
环境科学
✓ 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）