APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
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IF 24.319
Yangyang Zhou,Chen Chen,Qiling Li,Yanbo Liu,Ting Wei,Youzhen Liu,Zebing Zeng,Darren Bradshaw,Bing Zhang,Jia Huo
Hydrogenation of unsaturated biomass in a control manner is highly desirable but challenging, especially under mild conditions. We here report selective hydrogenation of α,β-unsaturated aldehydes (UALs), featuring a precise control of all potential products by adjustment of the role of ammonia borane (AB) in transfer and/or catalytic hydrogenation. The hydrogenation can be readily operated in neat water without using any external H 2 -source, because AB as the H 2 -source is favorable in aqueous solution. Impressively, unsaturated alcohols are prepared in 100% conversion by the room-temperature transfer hydrogenation of UALs with AB, while saturated aldehydes are obtained in 100% conversion and > 90% selectivity with high activity ( i.e ., turnover frequency = 0.98 s −1 for cinnamaldehyde), by the catalytic hydrogenation with H 2 released from AB and Pd immobilized on two-dimensional metal organic layer. On the other hand, UALs can be completely converted into the saturated alcohols through a combination of transfer and catalytic hydrogenation in one pot. This strategy can be extended to more than 8 types of UALs, and provides a facile way to fine-control the selective hydrogenation of unsaturated compounds with competing bonds.
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MICROPOROUS AND MESOPOROUS MATERIALS
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2022
·
IF 5.876
Yanghuan Huang,Haocheng Zhang,Lou Gao,Tianlan Yan,Yueer Yan,Yahong Zhang,Yi Tang
A series of Zr–Al-MWW zeolites with different Zr state and layer-stacking structure are successfully synthesized via direct grafting zirconocene dichloride onto the external silanols of three kinds of MWW zeolites, i.e. MCM-22 with multilayered structure, ITQ-2 (through layer delaminated route) and OL-MWW (by direct hydrothermal synthesis) with oligolayered structure. The structure, porosity and state of grafted Zr species are distinctly different among the three Zr–Al-MWW zeolites. Zr-OL-MWW possesses the highest content of single Zr atoms with an ideal micro-meso-macro pore system, while Zr-MCM-22 and Zr-ITQ-2 contain two kinds of Zr species (ZrO 2 clusters and single Zr atoms) coexisting in various proportions. The high dispersion of single Zr atoms on OL-MWW can be assigned to the large amount of external silanols of OL-MWW. The as-prepared three bi-functional Zr–Al-MWW zeolites are used for the cascade Meerwein-Ponndorf-Verley (MPV) reduction and etherification (ETH) reaction. Among them, Zr-OL-MWW shows dramatically higher conversion of cinnamaldehyde and yield of 1-cinnamyl 2-propyl ether than Zr-MCM-22 and Zr-ITQ-2, owing to the higher catalytic activity of Lewis acid centers from single Zr atoms, as well as more integrated framework Al sites as Brønsted acid centers with good accessibility. This study offers a simple and efficient strategy to construct Lewis-Brønsted acidic zeolites with exposed heteroatom sites and integrated framework structure, which will provide especial potential in the catalytic conversion of macromolecules.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2022
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IF 7.139
Qianqian Zhang,Yifan Sun,Wei Li,Jinli Zhang,Yan Fu
Selective hydrogenation of α, β-unsaturated aldehydes has always been a hot research topic owing to favorable thermodynamics in C C hydrogenation. In this work, a series of Pd/SnO 2 nanocatalysts were facilely synthesized under mild conditions, via the reduction of Na 2 PdCl 4 by dimethylaminoborane. Under galvanostatic electrolysis at 3.33 mA cm −2 for 8 h, the selective conversion of cinnamaldehyde (CAL) was achieved over Pd/SnO 2 -coated carbon fiber in neutral phosphate buffer, giving the cinnamyl alcohol (COL) selectivity of 78.85% at the conversion of 84.88%. The Pd/SnO 2 nanocatalysts outperform commercial Pd/C catalysts, showing high COL selectivity and faradaic efficiency. The cathodic reduction potential of CAL over Pd 4·3 /SnO 2 occurs at −0.92 V. The SnO 2 support is beneficial to promote the C O adsorption of CAL and lower the HER activity of Pd nanocatalysts, thereby contributing to superior activity of Pd 4·3 /SnO 2 for selective hydrogenation of CAL.
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CHEMOSPHERE
·
2021
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IF 7.086
Xiaoping Liu,Yunbo Zhai,Guangli Liu,Xiangmin Liu,Bei Wang,Zhexian Wang,Ya Zhu,Yuwei Fan,Haoran Shi,Min Xu
Without extra adjustment of pH, the effects of cupric ions (Cu(II)) and hydrogen peroxide (H 2 O 2 ) alone or in combination on sludge dewatering were studied. It showed good dewatering capability after treated by Cu(II) and Cu(II)/H 2 O 2 , which indicated by the capillary suction times (CST) decreased from 120.8 ± 4.7 s (control) to about 40 s, and the water content (Wc) of sludge cake dropped by about 10%. The results showed that the extracellular polymeric substances (EPS) were destroyed, which characterized by a significant decrease in the biopolymers’ concentrations in tightly-bound EPS. Meanwhile, more rough and porous microstructures and higher zeta potentials were obtained after conditioned. Based on the changes of physicochemical properties of sludge, the variations of EPS, and the identification of reactive species, two distinct mechanisms of improved sludge dewatering were postulated. As for Cu(II) treatment, it was mainly due to the surface charge neutralization, strong cytotoxicity of Cu(I) produced by intracellular reduction of Cu(II), and pH decline caused by Cu(II) hydrolysis that improved sludge dewatering performance, which could be noted as a “non-radical pathway”. When in combination with H 2 O 2 , hydroxyl radicals (·OH) produced by Cu(II)-catalyzed Fenton-like process played a dominant role in degrading sludge flocs and EPS, which could be regarded as a “radical pathway”.
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JOURNAL OF MATERIALS SCIENCE
·
2022
·Vol. 57
·期 5
·3168-3182
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IF 4.682
Tian Fuping,Zhang Mengjie,Zhang Xinchi,Chen Xiao,Wang Jinliang,Zhang Yifu,Meng Changgong,Liang Changhai
Hydrogenation of cinnamaldehyde (CAL) to cinnamyl alcohol (COL) or hydrocinnamaldehyde (HCAL) with high selectivity has important industrial value. Previous studies have shown that nickel-based catalysts are highly active and favor the selectivity to HCAL. However, Ni in metallic state is so active that most of nickel-based catalysts need to be pre-reduced before use. In this paper, a stable Ni–C catalyst was prepared by simple pyrolysis of Ni-BTC and systematically characterized. The results showed that metallic Ni nanoparticles were uniformly dispersed and encapsulated in the carbon layer, which protects the metallic Ni from oxidation. Therefore, the Ni–C catalyst can be directly used in CAL hydrogenation without pre-reduction. The catalyst Ni-C-600 achieved 92.5% selectivity to HCAL at 96.2% conversion of CAL at 120 °C under 2 MPa H 2 for 6 h with a poor reusability in isopropanol (IPA), while the catalytic performance and reusability were evidently enhanced (HCAL selectivity ~ 94%, CAL conversion ~ 99% in five consecutive runs for 4 h) in a solvent containing water and IPA. This study provides a facile and low-cost method to prepare effective Ni-based catalysts displaying excellent catalytic activity with high HCAL selectivity and stable reusability in CAL hydrogenation. Graphical abstract
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EUROPEAN FOOD RESEARCH AND TECHNOLOGY
·
2021
·Vol. 247
·期 11
·2687-2698
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IF 2.998
Liu Chen,Long Huali,Wu Xingdong,Hou Jinjun,Gao Lei,Yao Shuai,Lei Min,Zhang Zijia,Guo De-an,Wu Wanying
Cinnamomum verum and Cinnamomum cassia are widely used as spice and herbal medicine around the world. However, it is challenging to differentiate and make a quality evaluation for both Cinnamomum types due to their similarities in morphological features and general chemical composition using traditional analytical methods. In this study, a simple and efficient method was developed for the comprehensive evaluation of the two Cinnamomum, together with Cassia twig, by combining UPLC fingerprint analysis combined with quantitative analysis using two internal standards for the determination of multiple components (TSDMC). The content of 9 components (procyanidin B2, cinnamtannin B1, coumarin, 2-hydroxycinnamaldehyde, cinnamyl alcohol, cinnamic acid, cinnamaldehyde, 2'-methoxycinnamaldehyde, and eugenol) in samples was determined using reliable relative conversion factor factors that were obtained using procyanidin B2 and cinnamic acid as two internal reference standards. The quantitative results combined with chemometrics analysis were employed to identify these samples. This simple and reproducible method revealed great differences among the three Cinnamomum in their chemical composition and provides a promising method for accurate differentiation and quality evaluation for the three Cinnamomum.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2021
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IF 7.312
Yunchang Fan,Hui Luo,Chunyan Zhu,Wenjin Li,Di Wu,Hongwei Wu
This work synthesized a series of hydrophobic natural alcohols based deep eutectic solvents (NADESs). These NADESs exhibited high extraction ability for quinine. The NADESs with lower viscosity and stronger hydrogen bond accepting ability ( β ) had stronger extraction ability. Quinine acted as hydrogen bond acceptor (HBA) for the hydrogen bonding between quinine and NADESs. The extraction efficiency of NADESs for quinine was higher than ionic liquid (IL), trichloromethane and ethyl acetate. After extraction, the NADES phase could be reused and quinine could be recovered from NADES phase via back extraction with 1.0% acetic acid aqueous solution as extraction solvent. The NADESs have the advantages of ease of preparation and high atom-economy and may be promising solvents for the extraction of bioactive compounds from natural sources compared with ionic liquids and conventional organic solvents.
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MATERIALS CHEMISTRY AND PHYSICS
·
2020
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IF 3.408
Tao Guo,Ting Xu,Wentao Xia,Andrew J. Carrier,Li Wang,Xu Zhang
We report herein, double quantum dot composites of graphene oxide and CuO (GOQD-q-CuO), formed by a low-temperature solution process, possess enhanced haloperoxidase (HPO)-like catalytic activity, which catalyze the oxidation of Cl − by H 2 O 2 to generate reactive chlorine species (RCS). A sensitive and selective colorimetric sensor was then developed via the oxidation of 3,3ʹ,5,5ʹ-tetramethylbenzidine (TMB) by the GOQD-q-CuO catalytic system through the generation of RCS for H 2 O 2 and glucose detection, with detection limits of 0.5 and 2.5 μM and linear ranges between 2.5–200 and 5–400 μM, respectively. This sensor was further applied to glucose detection in clinical serum samples showing no significant differences with the hexokinase method. Additionally, we demonstrate that the GOQD modulates the catalytic activity of q-CuO by reversing its zeta potential , producing an overall negatively charged surface, therefore GOQD-q-CuO has much higher affinity than CuO to the positively charged chromogenic substrate TMB, yielding higher HPO-like activity. Moreover, the presence of Cl − accelerates electron transfer to facilitate Cu 2+ reduction to Cu + on the GOQD-q-CuO surface, speeding up the overall catalytic reaction for the RCS generation, therefore, higher detection sensitivity was achieved.
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LANGMUIR
·
2021
·
IF 3.882
Hongbo Yu,Jihao Zhao,Chunzheng Wu,Bo Yan,Shuangliang Zhao,Hongfeng Yin,Shenghu Zhou
Decoration of noble metals with transition-metal oxides has been intensively studied for heterogeneous catalysis. However, controllable syntheses of metal–metal oxide heterostructures are difficult, and elucidation of such interfaces is still challenging. In this work, supported IrCo alloy nanoparticles are transformed into supported Ir–CoOx close-contact nanostructures by in situ calcination and following selective reduction. Relative to Ir/Al2O3, Ir–CoOx/Al2O3 shows greatly enhanced activities for the hydrogenation of furfural derivatives to the corresponding furfuryl alcohol derivatives with more than 99% selectivity and demonstrates significantly improved activities and selectivity for hydrogenations of α,β-unsaturated aldehydes to α,β-unsaturated alcohols. The modification of Ir surfaces with CoOx prevents Ir nanoparticles from growing, achieving high thermal and catalytic stabilities. Theoretic calculation suggests that the better catalytic performance of Ir–CoOx/Al2O3 is ascribed to the Ir–CoOx interaction, which promotes the absorption of furfural as well as desorption of furfuryl alcohol, resulting in enhanced catalytic activities.
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APPLIED ORGANOMETALLIC CHEMISTRY
·
2020
·Vol. 34
·期 8
·e5697
·
IF 3.14
Yingpeng Huo,Jiwen Hu,Yuanyuan Tu,Zhenzhu Huang,Shudong Lin,Yangfei Hu,Chao Feng
An imidazolyl Schiff base-containing periodic mesoporous organosilica (PMO) was synthesized via co-condensation reactions between a newly prepared bis (imidazolyl)imine-bridged bis silane and tetraethyl orthosilicate in the presence of cetyltrimethyl ammonium bromide as a soft template. The resultant as-synthesized PMO was then employed as a solid support for platinum catalysts. This complex was fully characterized via various techniques including FTIR, solid-state 13 C NMR, and 29 Si-NMR spectroscopy, as well as N 2 adsorption/desorption analysis, X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), scanning electron microscopy (SEM), and transmission electron microscopy (TEM) methods. In addition, the catalyst was proven to efficiently mediate hydrosilylation reactions between olefins and hydrosilanes, and it can be reused for at least five cycles without significant loss of activity.
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DIAMOND AND RELATED MATERIALS
·
2022
·
IF 3.806
Shurui Xu,Baoqiang Lin,Qihang Huang,Wenting Qiu,Wenqian Yuan,Weirui Xu,Xingfeng Xue,Guoyu Zhong,Wenbo Liao,Wenlong Wang,Xiaobo Fu
Oat-derived N-doped carbon with tunable N content (OA-NCs) were synthesized and applied in alcohol oxidation to selectively produce aldehyde. OA-NCs exhibited unexpectedly high performance in the oxidation of benzyl alcohol, cinnamyl alcohol and furfuryl alcohol. N species were characterized to interpret its promoting effect on their catalytic activity . Oxidation activity of pyridinic N in OA-NCs was sensitive to their structure while reactivity assessment disclosed it was more active to convert alcohols in presence of Fe 3+ , rather than pyrrolic-N or graphite-N. The superoxide radical was evidenced as the most reactive oxygen species in this reaction. The strong metal-support interaction (MSI) between pyridinic N and Fe 3+ , indicated by DFT calculation, was determined to be critical for the high activity of OA-CNs catalysts. The present work provides the insight into the positive effect of N-metal interaction in carbon materials on O 2 activation and explores a green pathway for the selective production of aldehydes.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Rong Zhang,Liancheng Wang,Jingzhao Ren,Changchen Hu,Baoliang Lv
The confinement effect known as efficient strategy to enhance the heterocatalytic activity and stability, but a clear view regarding the role of encapsulated overlayers is far from convincing at present, especially, the penetration of substrates with different size. Herein, the experimental evidence about the impacts of BN overlayers on hydrogenation is obtained over Co@BN/BN model catalysts with tuned thinness, in which BN overlayers encapsuled Co particles that dispersed on the defective BN supports, fabricating by the nitridizing of ball-milled BN microplates under NH 3 atmosphere. The thinness and crystallinity of BN shells was simply tuned by controlling the pyrolyzed temperature (600–900 °C). The cinnamaldehyde (CAL) selective hydrogenation is taken as probe reaction due to (1) both larger CAL and small H 2 molecule involved simultaneously, (2) the middle C C and terminal C O bonds all involved. Combined with structural analysis, the results demonstrate that small H 2 molecule can penetrate into the metal-cover interface through the defect sites, then inner Co core dissociate it to atomic H, and the hydrogenation mainly resulting from the spillover of H atoms which occurred on the BN surface. As a result, the thickest BN shells (∼3.4 nm) with ordered-layer-lattice significantly hindered the adsorption and activation of CAL, also the longest H spillover distance led to the lowest activity of Co@BN/BN-900. Instead, Co@BN/BN-600 with merely 2 ∼ 3 overlayers presented the most efficient and highly chemoselective hydrogenation activity. The ultrathin but turbostratic BN overlayers provide more migrating sites also shortened the H spillover distance effectively, and the more favorable C O hydrogenation was also achieved driven by the steric hindrance effect of thinner BN shells. These observations provide new insights towards understanding of confined effect on catalysis process through the accurate regulation of BN shells properties.
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