Nano Research
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2022
·Vol. 16
·期 4
·5880-5886
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IF 10.269
Tian Zhengbin,Deng Xiaohui,He Ping,Wang Guang-Hui
Monolithic catalysts play a crucial role in various catalytic applications, e.g., chemical synthesis, energy conversion, and environmental treatment, but their catalytic efficiency is often limited by the restricted mass transfer and insufficient exposure of active sites. Herein, we present a dual-templating strategy to fabricate atomic Pt dispersed on monolithic N-doped mesoporous carbon nanowires (Pt 1 /NMCW) with abundant super-/macropores, which, as monolithic catalyst, exhibits high catalytic performance in hydrogenation of 4-nitrophenol (4-NP). During synthesis, triblock copolymer (Pluronic F127) is employed as a primary soft template to generate the mesoporous structured carbon nanowires to improve the accessibility of Pt single sites; KCl crystallite is used as a secondary hard template to create the super-/macropores, which are beneficial for enhancing the mass transfer efficiency. Thanks to the dual-templating strategy that creates the monolithic carbon nanowires with hierarchically porous structure, the obtained Pt 1 /NMCW shows highly enhanced catalytic activity in 4-NP hydrogenation, outperforming its analogue synthesized without using KCl as template and being comparable to the nano-powder catalyst (i.e., atomic Pt loaded on the N-doped carbon nanospheres, Pt 1 /NCS).
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Jiasheng Wang,Ying Zhang,Xiaonan Xu,Ming Bao
Halogenated arylamines are important intermediates for the synthesis of dyes, pesticides, herbicides, and other chemicals. One important way to prepare halogenated arylamines is catalytic hydrogenation of halogenated nitroarenes. Ni-based catalysts have been used in the hydrogenation of halogenated nitroarenes but suffer from low activity and dehalogenation side reaction. In this paper, Ni–CeO2/SiO2 heterojunction catalyst with a “raisin-bun” structure was prepared by reverse microemulsion. A built-in electric field and more oxygen vacancies were formed due to electron transfer from Ni to CeO2 as a result of their work function difference. The built-in electric field leads to the heterolytic cleavage of H2, thereby improving the hydrogenation activity. Oxygen vacancies preferentially adsorb and activate nitro groups, inhibiting the dehalogenation side reaction. Through the cooperation of built-in electric field and oxygen vacancy, synchronous enhancement of the activity and selectivity is obtained successfully. This finding provides a new view for the design of non-noble metal-based catalysts with high activity and selectivity.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2022
·
IF 4.326
Yebin Zhou,Ling Li,Yi Liu,Hongzheng Wang,Zhenlong Feng,Feng Feng,Qunfeng Zhang,Wucan Liu,Wenfeng Han,Chunshan Lu,Xiaonian Li
Most of the catalytic hydrogenation reactions take place under high temperature, high pressure, and high corrosion, which poses a challenge to the activity and stability of hydrogenation catalysts. Herein, an acid resistant and strawberry-like metal–carbon sphere (M/SCS) as a robust hydrogenation catalyst was synthesized by a one-step method. Self-assembled metal nanoparticles gather and are embedded on the surface of the carbon sphere prepared by the carbonization of phenolic resin. By means of the surrounding carbon layer, the acid resistant capability is orders of magnitude intensified compared to traditional commercial catalysts. Over 91.5% and 100% metals of Pd/SCS7 and Pt/SCS7 remain as the catalyst in hydrochloric acid (36–38 wt %), while less than 44.6% and 37.5% metals remain of commercial Pd/AC and Pt/AC. In addition, the sizes are controlled in the range of 11 to 18 nm for metal particles and 400 to 1600 nm for carbon spheres by adjusting the conditions of phenolic aldehyde condensation. N atoms anchored on the carbon spheres with high dispersion can improve electron density on metal particles. M/SCS exhibits both excellent stability and high catalytic performance in the hydrogenation reactions.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Zhijun Li,Mingyang Zhang,Xiuli Dong,Siqi Ji,Lili Zhang,Leipeng Leng,Honghong Li,J. Hugh Horton,Qian Xu,Junfa Zhu
The realization of efficient and fully controllable synthesis of single atom catalysts is an exciting frontier, yet still challenging in the modern catalysis field. Here we describe a straightforward high-temperature quenching approach to precisely construct isolated palladium atoms supported over cubic indium oxide, with individual palladium atoms coordinated with four neighboring oxygen atoms. This palladium catalyst achieves exceptional catalytic efficiency in the selective hydrogenation of nitrobenzene to aniline, with more than 99% chemoselectivity under almost 100% conversion. Moreover, it delivers excellent recyclability, anti-CO poisoning ability, storage stability, and substrate tolerance. DFT calculations further reveal that the high catalytic activity stems from the optimized electronic structure and the charge states of palladium atoms in the defect-containing indium oxide. Our findings provide an effective approach to engineering single atom catalysts at the atomic level and open the door to a wide variety of catalytic reactions .
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ACS Applied Nano Materials
·
2022
·
IF 6.14
Fan Yang,Hongbo Yu,Chunzheng Wu,Shiwei Wang,Tong Li,Hongfeng Yin
Supported Rh nanoparticles (NPs) exhibit excellent activity for the chemoselective hydrogenation of halonitrobenzenes (HNBs), but their selectivity to aromatic amines is not satisfactory due to the side reaction on the carbon–halogen bonds, and their recycling stability is limited due to the aggregation and the leaching of active component during the long-term usage. Herein, we design a yolk–shell-structured catalyst that consists of RhCu alloy cores and hollow/microporous carbon shells (HCS) to overcome these problems. The obtained RhCu@HCS catalyst with a Rh/Cu ratio of 1:1 showed good activity, selectivity, and stability in the hydrogenation of p-CNB (p-chloronitrobenzene) to produce p-CAN (p-chloroaniline) due to the synergistic effect between Rh and Cu. The protective carbon shells not only prevented the aggregation of metal NPs but also allowed the reactants to diffuse freely across the shells. Therefore, our research provides a general strategy to design highly efficient and stable hydrogenation catalysts.
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JOURNAL OF CHROMATOGRAPHY A
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2022
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IF 4.601
Ziqi Sun,Meiling Qi
This work presents the investigation of a novel CO 2 -based poly(ether-carbonate) copolymer, namely poly(propylene ether-carbonate)diol (PPCD), for gas chromatographic (GC) analyses. The PPCD column exhibited column efficiency of 4000 plates/m determined by naphthalene at 120 ℃ with the retention factor 6.23. Its separation performance was investigated by adopting a wide variety of analytes and isomers, including the isomer mixtures of alkanes, substituted benzene isomers with diverse groups, phenols and anilines, and the mixtures of organic solvents of high volatility, aliphatic amines and N-heterocycles. As a result, the PPCD column displayed distinctly higher resolving capability than the commercial columns described herein and achieved high column inertness towards acidic/basic analytes without involving any deactivation procedure. Additionally, it displayed excellent separation repeatability and reproducibility with the relative standard deviation (RSD) values less than 0.01% for within-day and in the range of 0.26% – 0.36% for between-day and 3.0% – 4.1% for between-column ( n = 4). Further, the PPCD column (30 m) was used to GC–MS analysis of the lemongrass essential oil and resolved more components well than the indicated commercial columns, evidencing its outstanding separation performance for analyses of complex samples. Up to date, the CO 2 -based poly(ether-carbonate) copolymers are not reported in the field of chromatography. This work demonstrates their promising future as a new type of selective and inert stationary phases for practical GC analyses.
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ACS Applied Nano Materials
·
2021
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IF 5.097
Hongbo Yu,Chunzheng Wu,Shiwei Wang,Tong Li,Hongfeng Yin
Modification of active metals with metal oxide modifiers has attracted considerable attention in heterogeneous catalysis due to their synergistic effect. However, a controllable synthesis of highly reactive and stable metal–metal oxide hybrid nanocatalysts is difficult. To solve this problem, presynthesized IrM (M = Fe, Co, and Ni) bimetallic nanoparticles were initially confined in the mesopores of SBA-15 and were then in situ transformed to Ir-MOx hybrids. The obtained Ir-MOx/SBA-15 nanocatalysts show superior activity and selectivity in the hydrogenation of substituted nitroaromatics to corresponding aromatic amines compared to Ir/SBA-15. Among these Ir-based catalysts, Ir-FeOx/SBA-15 exhibits the highest activity and selectivity and has a wider substrate scope due to the interaction between Ir and FeOx. Therefore, our research provides a way to design reactive and stable hydrogenation catalysts.
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CHEMISTRY-A EUROPEAN JOURNAL
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2021
·Vol. 27
·期 41
·10666-10676
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IF 5.236
Peng Zhang,Shaonan Xu,Yan Wang,Wei Zhang,Wenqing Li,Cundi Wei,Peiping Zhang,Shiding Miao
Graphical One man‘s trash is another man‘s treasure : A novel template strategy allows fibrous struvite—a composite Pd/Mg 2 P 2 O 7 with a mesoporous structure and an ultrahigh surface area—to be synthesized from wastewater. The prepared Pd/Mg 2 P 2 O 7 nanowires showed excellent performance in the selective hydrogenation of nitrobenzenes. This strategy provided a new pathway for synthesizing highly efficient catalysts as well as a solution for alleviate eutrophic pollution caused by N- and P-containing substances in wastewater. A highly efficient heterogeneous catalyst Pd/Mg 2 P 2 O 7 was fabricated by combining palladium nanoparticles (PdNPs) and mesoporous Mg 2 P 2 O 7 fibers/rods. Mg 2 P 2 O 7 fibers with ultra-high specific surface area were prepared from struvite as templates, which were synthesized from waste water containing N- and P-containing pollutants. This strategy provided a novel pathway for developing advanced catalysts from eutrophication-polluted water. The composite Pd/Mg 2 P 2 O 7 showed brilliant performance in selective hydrogenation of nitro aromatics to give anilines. As an example of nitrobenzene hydrogenation, the conversion to aniline and selectivity were found to reach almost 100 % at a temperature of T =90 °C and under a pressure of P =2.0 MPa. The superior performance was found to originate from PdNPs, which were boosted by electron transfer afforded by the nanofiber Mg 2 P 2 O 7 supports. The favorable adsorption of withdrawing groups (−NO 2 ) was realized by synergistic effects between Pd and oxygen vacancies provided by pyrolysis of struvite. The catalyst remained stable after cycles of reuse with little degradation in catalytic performance.
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Catalysts
·
2021
·Vol. 11
·期 5
·543
·
IF 4.146
Zechen Liang,Mingkai Zhang,Sai Zhang,Yongquan Qu
Selective hydrogenation of halonitrobenzenes into haloanilines represents a green process to replace the environmentally unfriendly non-catalytic chemical reduction process in industry. However, this transformation often suffers from serious dehalogenation due to the easy break of carbon-halogen bonds on metal surfaces. Modulations of the electronic structure of the supported Pd nanoparticles on Lewis-basic layered double hydroxides have been demonstrated to promote catalytic activity and selectivity for hydrogenation of halonitrobenzenes into haloanilines. Mechanism studies suggest that Pd with the enhanced electron density not only improves the capability for hydrogen activation, but also generates the partially negative-charged hydrogen species to suppress the electrophilic attack on the carbon-halogen bond and avoid the dehalogenation.Keywords:Pd nanoparticles;hydrogenation;halonitrobenzenes;haloanilines
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DYES AND PIGMENTS
·
2021
·
IF 4.889
Wei Lang,Gengjinsheng Cheng,Rongpeng Peng,Qian-Yong Cao
A fluorescent poly (norbornene)-based copolymer probe P1 , which was obtained via ring-opening metathesis polymerization (ROMP) of a PEG-anchored norbornene monomer NB-PEG with a rhodamine-functionalized monomer NB-RB, has been designed and synthesized. Owing to its amphiphilic property, copolymer P1 self-assembles nanostructure aggregations in aqueous solution with a weak emission. Upon addition of ATP , visual color change from colorless to red and a large fluorescence enhancement were observed for the ring-opening of rhodamine spirolactam mechanism. This probe shows a good photostability, and has been successfully applied for imaging of ATP level in living SMMC cells.
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Journal of Physical Chemistry C
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2021
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IF 4.126
Pengchao Chen,Kaijie Li,Peijian Yan,Junyou Wang,Shenghu Zhou
In this work, Pd–FexOy hybrid nanoparticles encaged hollow mesoporous silica nanoreactors (Pd–FexOy@HMSNs) are synthesized, which features ∼3–4 nm Pd–FexOy hybrid nanoparticles inside ∼17 nm hollow cavities of ∼32 nm mesoporous silica nanoreactors. By employing Pd and Fe ions containing polymer micelles as templates for silica deposition, hollow mesoporous silica nanoreactors and the residence of functional nanoparticles inside hollow cavities are simultaneously obtained. Through adjusting the ratios of Pd2+/Fe3+ in micelles, various Pd–FexOy@HMSNs with different Pd/Fe ratios are synthesized and tested for reduction of nitroarenes with NaBH4. Relative to Pd@HMSNs, FexOy@HMSNs and their physical mixtures, Pd1–(FexOy)1/x@HMSNs illustrate a greatly enhanced catalytic performance for reductions of a series of substituted nitroarenes with NaBH4 to aminoarenes. The catalytic enhancement of Pd–FexOy@HMSNs is ascribed to the synergistic effect of Pd and FexOy as well as the confinement effect of functional nanoparticles inside hollow cavities.
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APPLIED CATALYSIS A-GENERAL
·
2020
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IF 5.006
Yueling Cao,Kangkai Liu,Chen Wu,Hepeng Zhang,Qiuyu Zhang
Inhibiting the dehalogenation is the main challenge when halogenated nitrobenzenes are hydrogenated using H 2 as hydrogen source by heterogeneous catalysis. Herein, the earth-abundant cobalt embedded into N-doped carbon (Co@CN) catalysts were fabricated via one-pot pyrolysis of tannic acid, Co(NO 3 ) 2 ·6H 2 O and melamine , which can function as a highly efficient non-noble-metal-based heterogeneous catalyst for selective hydrogenation of halogenated nitrobenzenes. Chloroanilines, bromoanilines, and iodoanilines, including all regioisomers, could be obtained with excellent selectivity (typically >99 %) at 60 °C under 1 MPa H 2 , at almost complete conversion of the substrates. Additionally, Co@CN demonstrated excellent catalytic stability and could be reused at least five times without obvious loss of catalytic activity and selectivity. Therefore, the Co@CN catalyst exhibits vast potential for future industrial application in the selective hydrogenation of halogenated nitrobenzenes.
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