Catalysis Science & Technology
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2024
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IF 4.4
Shan Hu,Yunfei Gao,Lu Ding,Xueli Chen,Weitong Pan,Fuchen Wang
Hydroformylation is an important reaction for aldehyde synthesis and requires ethylene and syngas (CO + H2) with the feedstocks. While these feedstocks are typically synthesized separately, it would be highly desirable to directly convert abundant ethane into ethylene and syngas in a single step. In this work, we loaded B2O3 onto perovskite La0.8Sr0.2FeO3 (LSF) and formed a core–shell structured catalyst, with B2O3 and Sr3B2O6 being the shell and LSF being the core. The shell structure can substantially inhibit deep oxidation of ethane into CO2 and the optimized La0.8Sr0.2FeO3@20B2O3 can achieve 69.2% ethane conversion and 88.8% ethylene + syngas selectivity at 700 °C with good stability, with a ratio of CO/H2 close to 1 : 1. The effects of reaction temperature, space velocity, B2O3 loading, and La/Sr were also investigated. This catalyst marks a promising progress for the direct oxidation of ethane and has good potential for industrial applications.
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
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2024
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IF 8.1
Xiuquan Li,Ziqiang He,Congbo Li,Dugang Kang,Jie Chen,Youhong Wang,Fei Wang,Song Huang,Zhien Zhang
Aiming at the resource utilization of CO 2 and the value-added catalytic conversion of ethane, different reducibility oxide carriers were used to study. Through catalytic reaction experiments, catalyst characterization and kinetic analysis , the interaction between reducible carriers and active metals and their regulation on the catalytic reaction performance of ethane with CO 2 were revealed. Fe 1.5 Ni 0.5 /CeO 2 has the highest ethylene selectivity of 87% near 650 °C, and is a good catalyst for the CO 2 -assisted ethane oxidative dehydrogenation to ethylene reaction. The strong interaction between the reducible CeO 2 and ZrO 2 carriers and active metals makes the Fe–O–Ce and Fe–O–Zr covalent bonds on the Fe 1.5 Ni 0.5 /CeO 2 and Fe 1.5 Ni 0.5 /ZrO 2 catalysts stronger than Fe–O–Ti and Fe–O–Al covalent bonds on Fe 1.5 Ni 0.5 /TiO 2 and Fe 1.5 Ni 0.5 /γ-Al 2 O 3 catalysts. The lattice oxygen on the reducible catalyst is more readily involved in the reaction. The strong interaction between the active metal and the carrier results in the reduction of the FeO x species and the formation of new active sites, resulting in a high reactivity of the catalyst. The mutually promoted redox cycle between the active species Fe 3+/2+ -Ni 2+/0 and the reducible carrier variable metal Ce 4+/3+ species improves the catalytic performance for the reaction of ethane awith CO 2 .
研究领域:
化学工程
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催化科学
✓ 已验证
DOI
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-11
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IF 14.7
Wang Pu,Zhang Xingyu,Shi Run,Zhao Jiaqi,Waterhouse Geoffrey I. N.,Tang Junwang,Zhang Tierui
The selective oxidative dehydrogenation of ethane (ODHE) is attracting increasing attention as a method for ethylene production. Typically, thermocatalysts operating at high temperatures are needed for C–H activation in ethane. In this study, we describe a low temperature ( < 140 °C) photocatalytic route for ODHE, using O 2 as the oxidant. A photocatalyst containing PdZn intermetallic nanoparticles supported on ZnO is prepared, affording an ethylene production rate of 46.4 mmol g –1 h –1 with 92.6% ethylene selectivity under 365 nm irradiation. When we employ a simulated shale gas feed, the photocatalytic ODHE system achieves nearly 20% ethane conversion while maintaining an ethylene selectivity of about 87%. The robust interface between the PdZn intermetallic nanoparticles and ZnO support plays a crucial role in ethane activation through a photo-assisted Mars-van Krevelen mechanism, followed by a rapid lattice oxygen replenishment to complete the reaction cycle. Our findings demonstrate that photocatalytic ODHE is a promising method for alkane-to-alkene conversions under mild conditions.
研究领域:
化学工程
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材料科学
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能源科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Catalysis
·
2021
·
IF 13.084
Yanliang Zhou,Yicong Chai,Xiaoyu Li,Zihao Wu,Jian Lin,Yujia Han,Lin Li,Haifeng Qi,Yiming Gu,Leilei Kang,Xiaodong Wang
Selective oxidative dehydrogenation (ODH) of light alkanes to alkenes over metal oxides usually obeys a redox catalysis cycle, where the release and recovery of lattice oxygen play a key role in catalytic performance. Therefore, it remains a challenge to prepare metal oxides with limited reducibility, such as TiO2, as a dominant active component rather than as a support or modifier in this process. Here, we find a significant increase of ethane ODH performance over a layered TiO2 (M-TiO2) catalyst, which is in situ evolved from a Ti3C2Tx MXene material during the reaction. The reactivity of this M-TiO2 is 4 times higher than that of P25 TiO2, with an excellent ethylene productivity of 15.4 gC2H4 gcat–1 h–1 that outperforms the previously reported catalysts. Experimental characterizations and theoretical calculations reveal the importance of Ti and oxygen vacancy defects over M-TiO2 on the conversion of C2H6. The Ti vacancy sites can stabilize the defective structure and increase the reducibility of lattice oxygen to reduce the activation energy barrier of ethane, while the oxygen vacancy sites facilitate the activation of O2 to recover lattice oxygen.
研究领域:
催化化学
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材料科学
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理论计算
✓ 已验证
DOI
高影响因子
Green Energy & Environment
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2022
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IF 12.781
Shuairen Qian,Yuxin Chen,Binhang Yan,Yi Cheng
High activity and productivity of MoVNbTeO x catalyst are challenging tasks in oxidative dehydrogenation of ethane (ODHE) for industrial application. In this work, phase-pure M1 with 30 wt% CeO 2 composite catalyst was treated by oxygen plasma to further enhance catalyst performance. The results show that the oxygen vacancies generated by the solid-state redox reaction between M1 and CeO 2 capture active oxygen species in gas and transform V 4+ to V 5+ without damage to M1 structure. The space-time yield of ethylene of the plasma-treated catalyst was significantly increased, in which the catalyst shows an enhancement near ∼100% than that of phase-pure M1 at 400 °C for ODHE process. Plasma treatment for catalysts demonstrates an effective way to convert electrical energy into chemical energy in catalyst materials. Energy conversion is achieved by using the catalyst as a medium.
研究领域:
催化化学
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材料科学
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能源转换
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
·
IF 19.503
Xin Tian,Chaohe Zheng,Haibo Zhao
The current study investigates Ce-modified SrFeO 3- δ oxygen carriers for oxidative dehydrogenation (ODH) of ethane coupled with CO 2 splitting in a chemical looping manner. During 39 cycles of redox testing over the sample of 0.2Ce/SrFeO 3 , up to 29% ethane conversion and 82% ethylene selectivity are achieved, and the CO generation in the subsequent CO 2 splitting step is 0.25 mmol/g. XPS characterization results indicate decreased Fe 2+ /(Fe 3+ +Fe 4+ ) ratio as well as increased active oxygen species proportion on the near-surface of Ce-modified samples, which are responsible for the improved activity of the 0.2Ce/SrFeO 3 in ethane ODH reaction. DFT calculations further reveal that the increased ODH activity of 0.2Ce/SrFeO 3 is due to the lower surface oxygen vacancy formation energy upon Ce promotion. Moreover, the higher resistance of lattice oxygen diffusion from the bulk to the surface is the main reason for the superior ethylene selectivity attained by the CO 2 -regenerated sample than that by O 2 regeneration.
研究领域:
化学工程
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
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