FUEL
·
2022
·
IF 8.035
Jia-Pei Guo,Fang-Jing Liu,Lei-Lei Bie,Xing-Gang Si,Yan-Hong Li,Ping Song,Nian Liu,Yun-Peng Zhao,Zai-Xing Huang,Jing-Pei Cao,Xian-Yong Wei
The utilization of lignin to produce high value-added chemicals is conducive to alleviating the fossil energy crisis. Herein, Ni nanoparticles supported on iron/nitrogen co-doped carbon was prepared by co-pyrolysis and solvothermal reduction method for catalytic hydrogenolysis (CH) of dealkaline lignin and its model compounds. The catalysts were prepared under different calcination temperature, N/C ratio and Ni loading, and the optimal catalyst was Ni 10% @Fe/NC 0.33 – 800 (calcination temperature: 800 °C, N/C ratio: 0.33, Ni loading: 10%) based the on the CH of benzyl phenyl ether (BPE). Ni 10% @Fe/NC 0.33 – 800 showed good catalytic performance on the selective cleavage of C-O bond of lignin and its model compounds. The BPE conversion reached up to 97.7% over Ni 10% @Fe/NC 0.33 – 800 under mild conditions (230 °C, 1 MPa H 2 , and 0.5 h) with toluene and cyclohexanol as major products. Catalyst characterizations suggest that N content affects the formation of NiFe alloy and the synergistic effect between Ni and Fe plays an important role in CH of BPE. Moreover, Ni 10% @Fe/NC 0.33 – 800 could promote the cleavage of C-O bonds in dealkaline lignin through CH and hence enhance producing aromatics such as phenols, aromatic ethers, and aromatic esters, among which phenols are the main aromatics with guaiacols predominant.
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SOLVENT EXTRACTION AND ION EXCHANGE
·
2023
·
IF 2
Dong Cao,Shuai Wang,Xin Ma,Jia Yang,Hong Zhong
Herein, a novel C=O–NOH-contained compound was synthesized and used in the extraction and recovery of copper from sulfate solution. Dodecyl phenyl ethyl hydroxamic acid (DPEHA) exhibited high selectivity to Cu(II) over the competing ions, and the separation factors (β) obtained were βCu/Zn = 227.370, βCu/Co = 199.094, βCu/Ni = 188.889, respectively. The separation effect was stronger than that of 2-hydroxy-5-nonyl acetophenone oxime. Meanwhile, extraction capacity of 0.10 g Cu(II) per gram DPEHA was reached, and the extracted Cu(II) can be stripped effectively. The investigation of extraction mechanism revealed that O atoms in C=O and O-H groups of DPEHA operate as active sites, which could powerfully chelate with Cu(II) by forming stable five-membered rings. The high copper extraction efficiency and selectivity associated with a simple synthesis of DPEHA make it to serve as the potential selective Cu(II) extractant, which also provide a novel insight for the research and development of economical Cu(II) extractants.
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CHINESE JOURNAL OF CATALYSIS
·
2013
·
IF 1.304
Qi SONG,Jiaying CAI,Junjie ZHANG,Weiqiang YU,Feng WANG,Jie XU
Phenethyl phenyl ether (PPE) was selected as a typical lignin model compound and hydrogenated and cleaved over two readily accessible nickel-based catalysts, which could be easily separated from the product mixture. The results revealed that the reduction of the nickel catalyst with gaseous hydrogen produced a species capable of achieving higher activity towards C-O-C bond cleavage compared to the Ru/C and Pd/C catalysts. The selectivity of the C-O-C bond cleavage over the Ni/C catalyst was 85%, and higher than the corresponding values in the Ru/C (40%) and Pd/C (69%) systems. Using the carbothermal reduction method for the production of the Ni/C-C catalyst, the conversion and selectivity levels reached 99%, with 40% of the benzene rings in PPE being reserved. In comparison, no benzene ring containing products wer observed over the noble metal catalysts. This difference was attributed to the interaction between the carbon support and the nickel nanoparticles. 摘要 研究了Ni基催化剂上木质素模型化合物苯基苯乙醚中C–O–C键加氢裂解性能. 结果表明, 14;Ni/C催化剂显示出优异的加氢裂解能力, 14;苯基苯乙醚的转化率达到99%以上. Ni/C催化剂的还原方法对裂解选择性有重要影响; 氢气还原制备的Ni/C-H催化剂上, 14;C–O–C键裂解选择性为85%. Ru/C和Pd/C催化剂上裂解选择性分别为40%和69%. 采用碳热还原方法制备的Ni/C-C催化剂, 14;可以实现高选择性加氢和裂解, 14;C–O–C键裂解选择性达到99%以上, 14;其中芳烃化合物收率为44%. 这可能与镍组分和载体碳之间的相互作用有关.
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APPLIED ORGANOMETALLIC CHEMISTRY
·
2013
·Vol. 27
·期 6
·337-340
·
IF 2.011
Junyu Dong,Tianbin Li,Chuan Dai,Wen Weng,Xinghua Xue,Yuyu Zhang,Qingle Zeng
A straightforward, protecting-group-free protocol for the synthesis of chiral 6-substituted and 6,6’-disubstituted binols (binol = 1,1’-bi-2-naphthol) by palladium-catalyzed hydroxylation, C–N and C–O coupling of chiral 6-bromo- and 6,6’ -dibromo-1,1’-binaphthols is developed. The protecting group free palladium-catalyzed hydroxylation, C–O and C–N cross-coupling protocol affords a straightforward and general method for the synthesis of chiral 6-substituted and 6,6’-disubstituted binols with good yields, avoiding the tedious procedures of introduction and removal of protecting groups. Copyright © 2013 John Wiley & Sons, Ltd.
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Catalysis Science & Technology
·
2023
·Vol. 13
·期 6
·1748-1754
·
IF 5
Shaoyuan Guo,Xinli Tong,Lingwu Meng,Guobao Yang
Selective oxidative C–C and C–O bond cleavage is of significance to the efficient utilization of biomass and biomass-derived platform compounds. In this work, the selective oxidative cleavage of C–C and C–O bonds has been developed with an iron-based catalyst (Fe–N–C) in the presence of molecular oxygen. Specifically, the β-O-4 lignin model compound was successfully converted to phenol and methyl benzoate in a methanol solvent, where the substrate conversion was 95.0% and the yields of phenol and methyl benzoate were 94.9% and 63.7%, respectively, when the reaction was performed with the Fe–N–C-850 catalyst at 120 °C for 4 h. Also, the oxidative transformations of other lignin models to phenols and methyl benzoates were achieved. Further investigations showed that the existence of the Fe3C phase in the catalyst plays an important role in the aerobic oxidative cleavage of C–C and C–O bonds in the β-O-4 lignin model.
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CARBON
·
2023
·
IF 10.9
Zhou Yang,Jin Zhang,Changfeng Wang,Hanzhong Cui,Li Yang,Huiyan Zhang,Renguo Guan
Graphene has been recognized as reinforcement and/or protective coating for metal materials due to its unique electronic, mechanical properties and chemical inertness . Challenges of graphene agglomeration and weak graphene/metal interfacial bonding still exist during preparation. Here we report a novel method combining capillary-assisted self-assembly with nascent hydrogen reduction technique to one step coat Al foil with layered-stacking graphene. Al foil constructed slit is filled with graphene oxide (GO) suspensions and the generation of nascent hydrogen occurs at the GO/Al interface. The capillary force drives the GO flakes to layer-by-layer assemble on Al foil, as well as increases the reduction depth of GO. X-ray photoelectron spectroscopy (XPS) reveals that the reduced GO (rGO) binds with Al is not just through van der Waals forces, but with a strong interaction of developing C–O–Al bonds. The hydroxyl groups on GO plays an essential role in the formation of such C–O–Al configuration. Al foil coated with rGO through this capillary-assisted self-assembly with nascent hydrogen reduction method show good corrosion resistance compared to the pristine Al and directly drop-casted GO on Al. The proposed method can be readily applied to the fabrication of graphene/metal composites with improved interfaces.
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CRYSTAL GROWTH & DESIGN
·
2020
·
IF 4.089
H. Liu,X. Yang,S. Cao,F. Yu,S. Long,J. Chen,M. Zhang,S. Parkin,T. Li,Z. Yang
A series of N-phenyl-2-hydroxynicotinanilides (PHNAs) have been synthesized, and their crystal structures have been investigated. The identity of these compounds is revealed to be the tautomer of PHNAs, i.e., 2-oxo-1,2-dihydropyridine-3-carboxylic acid phenylamides, compounds with both amide and lactam functionalities. Among these compounds, those with no or negligible steric hindrance take a near planar conformation and form lactam–lactam dimers, not the widely observed amide NH···O═C hydrogen bond chains, while those with steric hindrance take a twisted conformation and form an amide NH···O═C (lactam) hydrogen bond. A succinct theoretic study combining conformational analysis and molecular electrostatic potential surfaces (MEPS) survey provided a reasonable explanation of the formation of these two different hydrogen bond motifs.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Jingjing Tang,Hongchao Li,Xuan Zhang,Jieshu Qian,Bingcai Pan
Fe-based metal–organic frameworks (MOFs) have garnered significant attention as catalysts for heterogeneous Fenton reactions, while the limited efficiency of the Fe(III)/Fe(II) redox cycle hinders their widespread use in wastewater treatment. Herein, we successfully incorporated carbon nanotubes (CNTs) into MIL-101(Fe) to modulate the coordination environment of Fe for achieving better catalytic activity. The MIL-101(Fe)/CNTs/H 2 O 2 system shows outstanding performance in degrading various pollutants, with the catalytic activity of the MIL-101(Fe)/CNTs composites (98.8%) significantly surpassing that of MIL-101(Fe) alone (26.4%) or CNTs alone (3.5%). Multiple experimental findings suggest that this synergistic effect is primarily attributed to the C-O-Fe bridge bonds resulting from the interaction of surface carboxyl groups on CNTs with Fe in MIL-101(Fe). This unique coordination structure accelerates the redox cycle of Fe(III)/Fe(II), thereby promoting the generation of hydroxyl radicals (HO • ). Furthermore, the MIL-101(Fe)/CNTs composites demonstrate excellent reusability and stability, maintaining effectiveness over a wide pH range from 3.0 to 6.5. This study provides new insights into regulating the microstructure of Fe-based MOFs to enhance their Fenton catalytic activity.
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ACS Catalysis
·
2025
·
IF 13.1
Tingting Xiao,Jingrong Li,Jian Li,Qihang Gong,Peikai Luo,Xinluona Su,Haiyang Cheng,Chao Zhang,Fengyu Zhao
The hydrogenolysis of cellulose-derived 5-hydroxymethylfurfural is essential for the production of fuels and chemicals from biomass. Herein, we fabricated a phosphorus-doped Pd/P-TiO2 catalyst for the hydrodeoxygenation of 5-hydroxymethylfurfural to 2,5-dimethylfuran. A large number of defects and electron-deficient Ti4+ sites (dTi4+) were formed by doping phosphorus into the TiO2 support, which could promote hydrogen spillover and reactant adsorption. Moreover, the spilled active hydrogen induced the formation of P–O(H)-dTi4+, which acted as a “Brønsted acidic site” to promote the activation of C–O bonds. Consequently, the Pd/P-TiO2 catalyst exhibited superb activity for the hydrodeoxygenation of 5-hydroxymethylfurfural to 2,5-dimethylfuran at mild conditions of 150 °C under 1 MPa H2.
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JOURNAL OF CATALYSIS
·
2025
·
IF 6.5
Xiaofei Liu,Daiyu Song,Yunyun Liu,Zhao Huang,Xinyao Wang,Kezhi Wang,Yuxin Yang,Yihang Guo
The cleavage of C–O bonds in biomass-derived carbohydrates is of great significance for the conversion of biomass to chemicals and fuels. We demonstrated that various F127-directed covalent triazine frameworks functionalized by sulfonic acid-based ionic liquids ([C 3 N][OTf]-FCTF) were synthesized by a two-step synthesis process. The interesting morphology of spherical nanofiber of the [C 3 N][OTf]-FCTF(0.25)-10 catalyst was obtained by carefully adjusting the usage of both F127 and ethanol in the synthetic system. The 5-hydroxymethylfurfural synthesis reaction parameters of were first optimized using the [C 3 N][OTf]-FCTF(0.25)-10 via response surface methodology. The [C 3 N][OTf]-FCTF(0.25)-10 exhibited high catalytic activity, and outperformed other CTF-based catalysts with different morphologies and commercial solid acids in the conversion of carbohydrates (e.g., fructose, inulin, sucrose and honey). This is due to the advantages of the loose spherical nanofiber, the rich N-containing units, the suitable Brønsted acid nature and the adjacent acid-base pairs on the surface of the catalyst. The high Brønsted acidity of [C 3 N][OTf]-FCTF(0.25)-10 played a positive role in the selective synthesis of levulinic acid from carbohydrates. The theoretical calculations demonstrated that discrepancies in electron cloud distribution between constructed acid-base pairs and N-rich groups in the catalyst could facilitate the cleavage of C–O bonds in fructose molecules. The Fukui function combined with experimental results elucidated the reaction pathways. The robust interaction between –[C 3 N][OTf] groups and frameworks ensured the excellent reusability of [C 3 N][OTf]-FCTF catalysts. This study will provide a novel approach for synthesizing CTF-based solid acids with controllable morphology, enabling the high-value utilization of carbohydrates.
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Catalysts
·
2022
·Vol. 12
·期 12
·1625
·
IF 4.501
Bo Chen,Zhi-Ze Cao,Zhi-Jun Diao,Liang-Qiu Huang,Si-Jia Zhao,Hong Yuan,Jia-Meng He
Hydrogenolysis via targeted depolymerization of C–O linkages is a techno-economic beneficial process for converting lignin into highly valuable chemicals and clean fuels. In this work, a macroporous silicalite-1 (S-1) array-supported Ru-Ni metallic phosphide composite (Ru-Ni12P5/S-15) was prepared as a catalyst and hydrogenolysis activity under relative mild conditions was investigated using a series of compounds containing ether linkages as lignin-related model compounds. The Lewis acid sites originating from the unreduced Ru species and the macroporous geometry of S-1 significantly influenced hydrogenolysis activity and product selectivity. Analysis of the mechanism demonstrated that both the aryl ether and aliphatic ether linkages were directly hydrogenated over Ru-Ni12P5/S-15. 2D-HSQC-NMR spectroscopy demonstrated that the ether linkages of lignin were efficiently cleaved by Ru-Ni12P5/S-15. Furthermore, the obtained liquid hydrogenolysis products are high value-added chemicals used for pharmaceutical production and can be facilely tuned via the reaction conditions.
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Surfaces and Interfaces
·
2026
·
IF 6
Aidi Xie,Wusong Geng,Chun Chen,Yunxia Zhang,Haimin Zhang,Guozhong Wang
A mesoporous SiO 2 -supported Ag catalyst co-modified with B 2 O 3 and amino groups (B/Ag@NH 2 −MS) was synthesized through the grafting of amino group onto silica and subsequent impregnation with 10 wt.% Ag and 5 wt.% B 2 O 3 . Density functional theory (DFT) calculations and Bader charge analysis showed that boron (B) doping triggered extensive electronic changes in the modified support. It implied that B atoms gained a partial positive charge, showing Lewis acidic nature, while nearby Ag atoms had a partial negative charge. This electronic redistribution led to a downward movement of the Ag d -band center and a decrease in the work function, which in turn modulated the binding energies of adsorbates and reduced the desorption barrier of MG. Such dual-site cooperation strengthened the adsorption and polarization of the DMO carbonyl group at the adjacent Ag and B sites, thus promoting the activation of the C = O bond. Moreover, the anti-sintering capacity of Ag nanoparticles could be ascribed to their efficient stabilization mechanism, resulting from the synergistic action of oxygen-bridged B/O/Ag species and –NH 2 functional groups.Consequently, it is noted that the catalyst is able to maintain a conversion of about 99% DMO and a selectivity of about 94% MG, and it was able to maintain a conversion rate of over 96% for >350 h. These observations highlight a dual-site electron synergy strategy for developing very active and long-lasting Ag catalysts for ester hydrogenation.
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