INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2024
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IF 3.8
Tianci Zheng,Yanfei Zhu,Rui Ma,Liguang Bai,He Yu,Shixi Zhao,Yufei He,Yanan Liu,Dianqing Li
Hydrogenation of unsaturated C≡C groups is a promising way to realize ethylene purification in petrochemical processes and produce value-added products. Gold catalysts are known to exhibit satisfactory selectivity toward olefins. However, it still remains a grand challenge to improve the activity and inhibit the heavy coke effect while balancing the selectivity. This article describes the construction of Cu vacancies at an abrupt surface over a Au–Cu alloy catalyst to effectively promote the activation and dissociation of hydrogen, thereby reducing the activation energy barrier. More importantly, the generation of abundant Cu vacancies contributes to the electronic interaction with the adjacent second metal to generate coordination unsaturated and electron-deficient Au species, which facilitates the desorption of product intermediates. Consequently, the activity and selectivity of the acid-etched Au3Cu1/TiO2 are much higher than those of the untreated Au–Cu and monometallic Au catalysts. This report opens up promising possibilities for engineering highly efficient heterogeneous gold catalysts.
研究领域:
催化化学
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材料科学
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石油化工
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
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IF 8.6
Hua Shuai,Junhui Liu,Yesong Teng,Xing Liu,Lingmin Wang,Hanting Xiong,Pengxiang Wang,Jingwen Chen,Shixia Chen,Zhenyu Zhou,Shuguang Deng,Jun Wang
Energy-efficient adsorptive separation shows great potential for the one-step production of high-purity ethylene (C 2 H 4 ) from ternary C 2 hydrocarbons. However, it remains a formidable challenge to fabricate high-performance adsorbents that exhibit simultaneous high selectivity (>2) towards acetylene/ethylene (C 2 H 2 /C 2 H 4 ) and ethane/ethylene (C 2 H 6 /C 2 H 4 ). Herein, we report a pillar-layered metal–organic framework, Ni(sdba)(dabco) 0.5 (H 2 sdba = 4,4′-sulfonyldibenzoic acid; dabco = 1,4-diazabicyclo [2.2.2] octane), for preferential trapping of C 2 H 6 and C 2 H 2 over C 2 H 4 . The abundant accessible binding sites endow Ni(sdba)(dabco) 0.5 with outstanding C 2 H 2 /C 2 H 4 (2.28) and C 2 H 6 /C 2 H 4 (2.47) selectivity with high C 2 H 6 (3.15 mmol g −1 ) and C 2 H 2 (4.41 mmol g −1 ) uptake among porous materials reported for one-step C 2 H 4 purification. Dynamic breakthrough experiments demonstrated the feasibility of producing high-purity C 2 H 4 (>99.9%) from C 2 H 2 /C 2 H 6 /C 2 H 4 gas-mixtures (1/1/1 and 1/9/90, v/v/v ) in a single step. Computational simulations reveal that the aromatic-rich pore spaces, which decorated with accessible interlayer uncoordinated oxygen atoms of sulfonyl groups and alkyl functionalities, can provide multiple C-H···O, C-H···π, and C-H···H interactions for selectively recognizing C 2 H 6 and C 2 H 2 over C 2 H 4 .
研究领域:
材料科学
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化学工程
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DOI
高影响因子
AICHE JOURNAL
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2025
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IF 4
Xiaoqing Wang,Ye Li,Xiaomin Li,Yong Wang,Feifei Zhang,Shishuai Li,Libo Li,Jinping Li,Jiangfeng Yang
Developing ethane (C 2 H 6 )-selective adsorbents is crucial for energy-efficient separation and the direct production of high-purity ethylene (C 2 H 4 ). While pure-silica zeolites show promise, their limited selectivity necessitates the exploration of alternative materials. Herein, we present AlPO 4 -17, an electrically neutral aluminum phosphate (AlPO) zeolite and isostructural analog of pure-silica zeolites. Featuring ultra-microporous structures and low-polarity surfaces, AlPO 4 -17 exhibits denser and stronger C−H···O interactions with C 2 H 6 than with C 2 H 4 . This results in the highest experimentally confirmed C 2 H 6 /C 2 H 4 selectivity (2.27) and C 2 H 6 adsorption heat (36.05 kJ/mol) among all reported C 2 H 6 -selective zeolites. Breakthrough experiments validate its superior C 2 H 6 /C 2 H 4 separation performance. Vacuum pressure swing adsorption (PSA) experiments demonstrate its practical efficiency under real-world conditions, while PSA simulations highlight its potential for enhanced recovery. As the first AlPO zeolite developed for C 2 H 6 /C 2 H 4 separation, AlPO 4 -17 offers valuable insights into the design of advanced C 2 H 6 -selective adsorbents, paving the way for more efficient industrial C 2 H 4 purification processes.
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DOI
高影响因子
Science Advances
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2022
·Vol. 8
·期 23
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IF 14.957
Peixin Zhang,Yao Zhong,Yan Zhang,Zhenliang Zhu,Yuan Liu,Yun Su,Jingwen Chen,Shixia Chen,Zheling Zeng,Huabin Xing,Shuguang Deng,Jun Wang
One-step separation of C 2 H 4 from ternary C 2 H 2 /C 2 H 4 /C 2 H 6 hydrocarbon mixtures is of great significance in the industry but is challenging due to the similar sizes and physical properties of C 2 H 2 , C 2 H 4 , and C 2 H 6 . Here, we report an anion-pillared hybrid ultramicroporous material, CuTiF 6 -TPPY, that has the ability of selective recognition of C 2 H 4 over C 2 H 2 and C 2 H 6 . The 4,6-connected fsc framework of CuTiF 6 -TPPY exhibits semi–cage-like one-dimensional channels sustained by porphyrin rings and TiF 6 2− pillars, which demonstrates the noticeably enhanced adsorption of C 2 H 2 and C 2 H 6 over C 2 H 4 . Dynamic breakthrough experiments confirm the direct and facile high-purity C 2 H 4 (>99.9%) production from a ternary gas mixture of C 2 H 2 /C 2 H 6 /C 2 H 4 (1/9/90, v/v/v) under ambient conditions. Computational studies and in situ infrared reveal that the porphyrin moieties with large π-surfaces form multiple van der Waals interactions with C 2 H 6 ; meanwhile, the polar TiF 6 2− pillars form C–H•••F hydrogen bonding with C 2 H 2 . In contrast, the recognition sites for C 2 H 4 in the framework are less marked.
研究领域:
材料科学
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化学工程
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物理化学
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吸附分离
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多孔材料
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DOI
高影响因子
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