CHEMICAL ENGINEERING JOURNAL
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2024
·
IF 13.3
Bowen Lu,Ziqiang Han,Xinyu Zhi,Liqi Zhang
NiFe 2 O 4 exhibits excellent redox properties and is widely applied in catalytic reactions. However, rapid inactivation under reaction conditions limited its industrial applications. In this study, CeO 2 -NiFe 2 O 4 composite catalysts were synthesized, and the Reverse Water Gas Shift (RWGS) reaction was measured to reveal its CO 2 hydrogenation performance under a high-temperature condition. NiFe 2 O 4 catalysts got deactivated after being reduced to Fe-Ni alloy at 700 °C, decreasing the CO 2 conversion rate. CeO 2 addition can significantly improve its high-temperature activity, and 20CeO 2 -NiFe 2 O 4 exhibited the best catalytic activity (80.85 %, 700 °C). The CeO 2 -confined maintained Ni-Fe alloy with a relatively small crystal size and larger specific surface area, supporting more active sites for CO 2 hydrogenation. CeO 2 addition induced higher oxygen vacancy concentration, enhancing CO 2 activation and formates species formed on 20CeO 2 -NiFe 2 O 4 , resulting in higher CO 2 conversion activity. In addition, 20CeO 2 -NiFe 2 O 4 maintained its catalytic stability for 50 h at 700 °C. The CeO 2 confined enhanced the high-temperature stability of Fe-Ni alloy. CeO 2 and formed CeFeO 3 dispersed in 20CeO 2 -NiFe 2 O 4 inhibited excessive aggregation of Fe-Ni alloy, and CeO 2 inhibited carbon deposition on Fe-Ni alloy, improving Fe-Ni alloy’s reaction stability under RWGS reaction conditions. CeO 2 confined may give insight into improving metal stability under high-temperature and reductive conditions in heterogeneous catalysis.
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
DOI
高影响因子
Catalysis Science & Technology
·
2021
·Vol. 11
·期 24
·7943-7954
·
IF 6.119
Hao Zhang,Xiaojing Song,Hao Sun,Zhenyu Lei,Shouxin Bao,Chen Zhao,Dianwen Hu,Wenxiang Zhang,Jingyao Liu,Mingjun Jia
Developing highly efficient and durable eco-friendly heterogeneous catalysts for the Friedel–Crafts acylation (FCA) reaction has been a long-term and significant target, yet remains a great challenge. Herein, a series of Fe–Ni alloy nanoparticles (NPs) encapsulated inside N-doped carbon spheres (FexNi1−x@NC) was rationally fabricated by pyrolyzing the Fe–Ni bimetallic metal–organic frameworks (BMOFs-FexNi1−x) to this end. Various characterization results demonstrated that FeNi alloy NPs (25 nm) covered by a thin carbon shell (5 nm) were uniformly distributed throughout the entire carbon-based composite. A number of oxidized metal species (Fe3+, Ni2+) are present on the surface of the inner bimetallic core, which should be the main source of catalytically active centers of the carbon-wrapped metal NP catalysts. The composition-optimized Fe0.8Ni0.2@NC with relatively higher positive surface charges exhibited the highest catalytic activity and excellent stability for the acylation of aromatic compounds with acyl chlorides. The density functional theory calculations revealed that the catalytic activity of the FexNi1−x@NC catalysts could arise from the electron transfer, i.e., from the outermost layer of the carbon shell to the inner positively charged Fe-based metal NPs, which can lead to a positive charge distribution (by acting as weak Lewis acid sites) on the external surface of the carbon-encapsulated metal NP catalysts. In this case, the external carbon shell can function as ‘chainmail’ to transfer the Lewis acidity (positive charge), and also to protect the inner metal core from the destructive reaction environment, thus resulting in the formation of highly efficient and durable FCA catalysts.
研究领域:
材料科学
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催化化学
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绿色化学
✓ 已验证
产品关联
DOI
高影响因子
Molecular Catalysis
·
2022
·
IF 5.089
Kuan Wang,Zhe Cao,Junlei Wang,Zhen-Hong He,Dan Wang,Rong-Rong Zhang,Weitao Wang,Yang Yang,Zhao-Tie Liu
The development of non-precious metal catalysts in heterogeneous catalytic processes is of great importance to the hydrogenation of quinolines for both theoretical and industrial applications. Herein, an effective non-precious metal catalyst, 58% Fe 4 Ni 6 Cu 5 /MCM-41, was developed to catalyze the hydrogenation of quinolines under the green and mild conditions, which can achieve 97.5% conversion and exceeding 98% selectivity to tetrahydroquinoline in solvent-free at low temperature of 50 °C. Moreover, the acceptable results of the reusability and gram scale-up experiments proved an industrial application potential of the as-prepared catalyst. Meanwhile, in cyclohexane system, 58% Fe 4 Ni 6 Cu 5 /MCM-41 catalyst can further realize a higher activity of the hydrogenation at a lower temperature of 40 °C, achieving 98.2% conversion and 98% selectivity to tetrahydroquinoline. The existence of Fe-Ni and Ni-Cu alloys in Fe 4 Ni 6 Cu 5 /MCM-41 catalyst was demonstrated by TEM, XRD, XPS, H 2 -TPD, and Raman spectroscopy. And, Fe-Ni and Ni-Cu alloys can be well dispersed onto MCM-41 molecular sieves. For Fe 4 Ni 6 Cu 5 /MCM-41 catalyst, quinoline molecules can be adsorbed by Fe 3+ species on the surface of Fe-Ni alloy through the coordination, while hydrogen molecules can be adsorbed and activated by Ni-Cu alloy. Under the synergism of Fe-Ni and Ni-Cu alloys, the highly effective and selective hydrogenation of quinolines was achieved at low temperature and in solvent-free system. The present approach offers a prospective idea for building non-precious metal catalysts to realize the effective hydrogenation of N-heterocyclic compounds under mild conditions.
研究领域:
催化化学
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材料科学
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绿色化学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Xu Pan,Junhong Wang,Ye Chen,Qing Wen,Cunguo Lin,Haiping Gao,Zhenghui Qiu,Liuqingying Yang
As a green conversion device, the electricity performance of microbial fuel cell (MFC) was mainly affected by the extracellular electron transfer (EET) process of the biofilm. This paper presented the fabrication and characterization of carbonized derivatives composed with alloy nanoparticles (NPs) derived from Zr-based metal organic frameworks, which exhibited biocompatibility and high electrocatalytic activity. As the results of bioanodes, the charge transfer resistance decreased from 5.60 Ω (Zr-C) to 0.61 Ω (Fe/Ni-Zr-C), and the exchange current density increased from 0.56 mA/cm 2 (Zr-C) to 1.40 mA/cm 2 (Fe/Ni-Zr-C). Electrochemical tests and density functional theory (DFT) confirmed that Fe-Ni alloy NPs promoted the rapid transfer of electrons within the electrode and improved the EET efficiency mediated with the flavin compounds. High throughput sequencing and PICRUSt verified the specific screening function of Fe-Ni alloy for electrogenic bacteria (mainly Geoalkalibacter) and the promoting effect on the expression of flavin-related proteins in biofilm. The maximum power density of Fe/Ni-Zr-C MFC (5.09 W/m 2 ) was higher than that of Ni-Zr-C (4.19 W/m 2 ), Fe-Zr-C (3.58 W/m 2 ) and Zr-C (3.09 W/m 2 ) MFCs. Fe/Ni-Zr-C material can act as an economical and high-performance bioelectrocatalyst to improve the power generation capability of MFC by improving EET rate and energy conversion efficiency of biofilm.
研究领域:
环境科学
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材料科学
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微生物学
✓ 已验证
DOI
高影响因子
Small
·
2021
·Vol. 17
·期 36
·2102002
·
IF 13.281
Hong Li,Xinxin Shu,Peiran Tong,Jihui Zhang,Pengfei An,Zhengxing Lv,He Tian,Jintao Zhang,Haibing Xia
In this work, Fe–Ni alloy nanoclusters (Fe–Ni ANCs) anchored on N, S co-doped carbon aerogel (Fe–Ni ANC@NSCA catalysts) are successfully prepared by the optimal pyrolysis of polyaniline (PANI) aerogels derived from the freeze-drying of PANI hydrogel obtained by the polymerization of aniline monomers in the co-presence of tannic acid (TA), Fe 3+ , and Ni 2+ ions. In addition, the optimal molar ratio of the TA, Fe 3+ , and Ni 2+ ions for synthesis of Fe–Ni ANC@NSCA catalysts are 1:2:5, which can guarantee the formation of carbon aerogel composed of quasi-2D porous carbon sheets and the formation of high-density Fe–Ni ANCs with an ultrasmall size between 2 to 2.8 nm. These Fe–Ni ANCs consisting of N 4 –Fe–O–Ni–N 4 moiety are proposed as a new type of active species for the first time, to the best of the authors’ knowledge. Thanks to their unique features, the Fe–Ni ANC@NSCA catalysts show excellent performance in oxygen reduction reaction with a half-wave potential ( E 1/2 ) of 0.891 V and oxygen evolution reaction (260 mV @ 10 mA cm −2 ) in alkaline media as bifunctional catalysts, which are better than the state-of-the-art commercial Pt/C catalysts and RuO 2 catalysts. Moreover, Zn–air battery assembled with the Fe–Ni ANC@NSCA catalysts also shows a remarkable performance and exceptionally high stability over 500 h at 5 mA cm −2 .
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
FUEL
·
2020
·
IF 5.578
Limo He,Song Hu,Xiaofei Yin,Jun Xu,Hengda Han,Hanjian Li,Qiangqiang Ren,Sheng Su,Yi Wang,Jun Xiang
Fe-modified Ni/Al 2 O 3 catalysts with Fe/Ni molar ratios of 0, 0.5, 1 and 2 were prepared to promote the co-production of H 2 and carbon nanotubes (CNTs) during steam reforming of toluene as a tar model compound. After the addition of Fe, toluene conversion increased from 55.1% of Ni/Al 2 O 3 to 73.6% of F1N1A (Fe/Ni ratio of 1), and H 2 yield over F1N1A reached the maximum of more than 2000 mmol/(g-cata). Multi-walled carbon nanotubes with average diameter of 10–30 nm were generated and follow tip-growth mechanism. Compared with Ni/Al 2 O 3 , the addition of Fe remarkably increased the amount and quality of CNTs which had longer length and less tortuosity. These dual promoting effects on H 2 and CNTs after the addition of Fe were attributed to the strong interaction between Ni and Fe in Fe-Ni alloy. Fe-Ni alloy had the high activity for the decomposition performance of toluene and H 2 O to generate more H 2 and intermediates for improving the reforming reaction. Meanwhile, the high catalytic decomposition activity supplied more carbon species and the formation of Fe-Ni alloy enhanced the generation of metal carbide for promoting CNTs growth. Besides, the deposition of amorphous carbon was suppressed and the interaction between Ni particle and catalyst support was weakened after the addition of Fe, which kept the activity of catalyst and promoted the tip-growth of CNTs.
研究领域:
催化
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材料科学
·
化学工程
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）