CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Qing-Shan Niu,Yi-Ran Du,Xin-Peng Guo,Jing-Wen Sun,Si-Ping Pang,Bao-Hua Xu
The Pd-catalyzed N-debenzylation of hexabenzylhexaazaisowurtzitane (HBIW) to tetraacetyldibenzylhexaazaisowurtzitane (TADBIW) has provided high yields (up to 90.0 %, 12 h) in batch reactors, however, several phase transition stages during the catalytic process disable the development of a continuous flow system. In this work, we designed Pd-WO m bifunctional catalysts (Pd-WO m /MO n ) for such a transformation under three-phase reaction conditions with high efficiency. Remarkably, TADBIW was obtained with a high yield of 82.5 % upon reacting for 6 h at 40 °C on Pd-WO m (5.0)/CeO 2 (Pd: 1.33 mol%). Experimental studies combined with theoretical analysis reveal the HBIW-to-TADBIW conversion is a stepwise hydrogenolysis-acetyldebenzylation process, wherein the initial hydrogenolysis of Ac 2 O turn over the catalysis. Importantly, the presence of highly dispersed WO m domains with proper size not only facilitates hydrogen spillover from Pd site to the adsorpted Ac 2 O but also accelerates the subsequent dissociation of *Ac 2 O(H), enabling reduction of the overall energy barrier for debenzylation.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2024
·
IF 3.8
Lian Duan,Hongda Zhang,Mengmeng Huang,Le Sang,Jisong Zhang
The coating materials of monolithic foam catalysts have a remarkable influence on the mass transfer and reaction process of packed bed reactors. However, the external mass transfer performance of micropacked bed reactors (μPBRs) based on the organic polymer-coated foam catalyst has not been investigated. This study explores the α-methylstyrene hydrogenation reaction and external mass transfer performance of μPBRs with a polydopamine (PDA)-coated foam catalyst. Pd/PDA/nickel foam has excellent α-methylstyrene hydrogenation activity and stability compared to Pd/Al2O3/nickel foam in μPBRs. The effect of pressure, gas and liquid superficial velocities, and pore size of foam packing on external mass transfer coefficient ((ka)OV) was investigated. The (ka)OV of the PDA-coated foam packing can reach 0.31–1.03 s–1, which shows a notable improvement over the Al2O3 coating. Furthermore, an empirical correlation equation for (ka)OV in μPBRs with PDA-coated foam packing is developed to provide a foundation for further design optimization and industrial applications.
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Chemical Engineering and Processing-Process Intensification
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2025
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IF 3.9
Shichao Su,Yaqiao Tian,Huifeng Li,Weiyao Yang,Hongda Zhang,Feng Liu,Le Sang
The micropacked bed reactor (μPBR) with monolithic catalyst hydrogenation technology has received widespread attention due to its high efficiency, continuous operation, and safety. In this study, the Pd/PDA/foam catalyst was prepared via impregnation method and vanillin (VL) hydrogenation was investigated in green water solution based on the μPBRs. The effect of operating temperature, pressure, the number of foam catalyst block, VL concentration, liquid and H 2 flow rate on VL conversion and VA yield was discussed. The highest conversion of VL was 99.4% and product yield of vanillyl alcohol (VA) reached 84.9% with 2.8 MPa, 120°C, 22 blocks of Pd/PDA/Ni foam catalyst, H 2 flow rate of 10 mL·min −1 and liquid flow rate of 0.1 mL·min −1 , and short reaction time (0.106 h) in μPBRs. The kinetic of hydrogenation VL to VA was established. The reaction rate constant and activation energy in μPBRs were from 0.63 to 1.39 min −1 and 16.94 kJ·mol −1 . The STY of VA in μPBRs was 0.0824 kg·L −1 ·h −1 ·g −1 , which was bigger than that of batch hydrogenation devices.
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MICROPOROUS AND MESOPOROUS MATERIALS
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2024
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IF 4.8
Ximei Sun,Feirong Wang,Jieqiong Wang,Hao Xiao,Qiang Kang,Yiqian Zeng,Qinglai Yang,Xiaofeng Tan
Designing the robust catalysts with a self-supported open structure and engineering surface would be beneficial for promoting intrinsic activity, increasing active sites, and enhancing electron/mass transfer during catalysis. The metallic aerogels (MAs) with hierarchical porous nanostructures and pure metal skeleton could be a favorable platform for fabricating high-performance catalysts. The introduction of an interface engineering strategy causes beneficial structural and electronic properties of MAs. Herein, the ionic liquid (IL) induced metallic Pd aerogels with well-defined nanowires are developed for the efficient catalytic reduction of 4-nitrophenol (4-NP) in the presence of NH 3 BH 3 . The engineered IL-Pd aerogels exhibit the integrated advantages of exceptional catalytic activities (including a high k value of 31.2 × 10 −2 s −1 and a high turnover frequency (TOF) of 320.4 h −1 ), acceptable costeffectiveness with a low NH 3 BH 3 concentration (n[NH 3 BH 3 ]/n[4-NP] of 120), remarkable cyclability, and noticeable longstanding stability. This work opens a new avenue for developing high-performance MAs with improved activity and durability.
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ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Xiaoxiao Wang,Yanmei Yang,Zhiqing Zhou,Yuling Zhong,Miaomiao Qin,Weiqing Wang,Weifeng Li,Bo Tang
5-hydroxymethylfurfural (HMF) is one of the most promising biomass-based chemicals that is used to produce many kinds of important compounds. Especially, the selective conversion of HMF to 5-hydroxymethyl-2-furancarboxylic acid (HMFCA), an important chemical feedstock, has high industrial significance but is technically challenging. In this study, we present a high-performance photocatalyst for selective oxidation of HMF to HMFCA. By integrating an ultrasmall amount of palladium (Pd) nanoclusters (1.12‰ in weight) on defective hexagonal boron nitride nanosheets (Pd/defective h-BN nanosheets (dh-BNs)), outstanding photocatalytic performance can be achieved, resulting in up to a 95% HMF conversion ratio with an 82% HMFCA selectivity. The performance is considerably higher than that of pristine dh-BNs and Pd on defect-free h-BNs. More importantly, this Pd/dh-BNs catalyst maintains a high catalytic activity after eight cycles, demonstrating robust catalytic stability. Density functional theory calculations indicate that Pd/dh-BNs can lower the energy barrier for HMF oxidation and facilitate the desorption of HMFCA, which contributes to the high selectivity catalytic performance. This study not only introduces a promising photocatalyst for sustainable chemical transformations but can also provide valuable insights into the design of advanced photocatalytic material for biorefinery applications.
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REACTIVE & FUNCTIONAL POLYMERS
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2011
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IF 2.546
Kan Zhan,Huanhuan You,Wenyu Liu,Jie Lu,Ping Lu,Jian Dong
A novel type of Heck reaction catalyst composed of hydrophilic interpenetrating polymer networks (IPNs) and palladium (Pd) nanoparticles was prepared by simultaneous crosslinking of polyvinyl alcohol and polyacrylamide . The mesh sizes of the IPNs are one order of magnitude smaller than the average sizes of the uniformly dispersed Pd nanoparticles, which functions well to stabilize Pd nanoparticles and prevent aggregation. The Pd particles in the IPNs can catalyze Heck coupling reactions with high activities and be recycled over 20 times, providing more sustainability than any other polymer-stabilized Pd catalyst reported in the literature. The confined reactions inside the IPN nanopores in neat water may provide a green route for C–C coupling reactions.
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Journal of Environmental Sciences
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2024
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IF 5.9
Qianyu Xu,Haoyang Fu,Jiyuan Gu,Liyu Lei,Lan Ling
The overuse of antibiotics and antitumor drugs has resulted in more and more extensive pollution of water bodies with organic drugs, causing detrimental ecological effects, which have attracted attention towards effective and sustainable methods for antibiotics and antitumor drug degradation . Here, the hybrid nanomaterial (g-C 3 N 4 @Fe/Pd) was synthesized and used to remove a kind of both an antibiotic and antitumor drug named mitoxantrone (MTX) with 92.0% removal efficiency, and the MTX removal capacity is 450 mg/g. After exposing to the hybrid material the MTX aqueous solution changed color from dark blue to lighter progressively, and LC-UV results of residual solutions show that a new peak at 3.0 min (MTX: 13.2 min) after removal by g-C 3 N 4 @Fe/Pd appears, with the simultaneous detection of intermediate products indicating that g-C 3 N 4 @Fe/Pd indeed degrades MTX. Detailed mass spectrometric analysis suggests that the nuclear mass ratio decreased from 445.2 (M + 1H) to 126.0 (M + 1H), 169.1 (M + 1H), 239.2 (M + 1H), 267.3 (M + 1H), 285.2 (M + 1H), 371.4 (M + 1H) and 415.2 (M + 1H), and the maximum proportion (5.63%) substance of all degradation products (126.0 (M + 1H)) is 40-100 times less toxic than MTX. A mechanism for the removal and degradation of mitoxantrone was proposed. Besides, actual water experiments confirmed that the maximum removal capacity of MTX by g-C 3 N 4 @Fe/Pd is up to 492.4 mg/g (0.02 g/L, 10 ppm).
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Advanced Science
·
2025
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IF 14.1
Xinyi Lu,Pingping Jin,Qianyun Tang,Min Zhou,Hanjie Xu,Chen Su,Lei Wang,Feng Xu,Min Zhao,Yongxiang Yin,Jinqiu Zhang,Zhen Jia,Xinrui Peng,Jie Zhou,Lu Wang,Yan Chen,Min Wang,Min Yang,Daozhen Chen,Yu Chen
Cervical cancer (CC) is a major health threat to women, with immunotherapies targeting the programmed death receptor 1/programmed death ligand 1(PD-1/PD-L1) axis showing promise but encountering resistance in a significant patient population. This resistance has driven a critical quest to uncover the underlying mechanisms. This study uncovers a novel metabolic axis involving the nicotinamide adenine dinucleotide (NAD + ) salvage pathway enzyme nicotinamide phosphoribosyltransferase (NAMPT) and the deacetylase Sirtuin 1 (SIRT1), which regulates PD-L1 expression and nuclear localization in CC. This axis may be a key factor contributing to the resistance observed in immunotherapy. This study reveals that PD-L1 overexpression in cancers is regulated by both transcriptional and post-transcriptional processes. Acetyl-proteomic analysis pinpoints SIRT1 as a central regulator in the deacetylation of histone H3 at lysines 27, which may influence PD-L1 subcellular distribution. This finding reveals the epigenetic control of immune checkpoint proteins by metabolic pathways, offering a new perspective on the regulation of PD-L1. The identification of the NAMPT/SIRT1 metabolic axis as a critical factor suggests that targeting this axis may enhance therapeutic responses.
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Surfaces and Interfaces
·
2024
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IF 5.7
Jingang Yao,Yang Zhao,Jing Liu,Guanyi Chen,Beibei Yan,Zhanjun Cheng,Jianzi Qi,Lei Wang
Herein, carbon nanotubes (CNTs) are acidified and M ( M = B or N) doped to support Pd nanoparticles (PdNPs) for upgrading to Pd/MCNT catalysts used in H 2 production from formic acid (FA). The characterization analysis demonstrates the support composition affects the electronic properties and size of PdNPs, thus impacting the performance of Pd/MCNTs. Among the assessed materials, Pd/BCNTs exhibit the largest specific surface area (128.1273 m 2 g −1 ) and smallest PdNPs particle size (6.28 nm). These properties result in significant improvements in FA conversion (41.67 %), and turnover frequency value (3451 h −1 ) compared to conventional Pd/CNTs (17.36 % and 564 h −1 , respectively). The study evaluates the service life and repeatability of Pd/BCNTs and analyzes the catalyst mechanism. This study filled the vacancy of acidification-modified and doped CNTs in Pd regulation, enhanced Pd's catalytic performance, and further supported FA as an H 2 storage material.
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Nanomaterials
·
2024
·Vol. 14
·期 21
·1690
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IF 4.4
Shihao Cui,Dejian Xu,Zhiyuan Wang,Libo Wang,Yikun Zhao,Wei Deng,Qingshan Zhao,Mingbo Wu
Palladium (Pd) catalysts play a crucial role in facilitating Suzuki cross-coupling reactions for the synthesis of valuable organic compounds. However, conventional heterogeneous Pd catalysts often encounter challenges such as leaching and deactivation during reactions, leading to reduced catalytic efficiency. In this study, we employed an innovative intercalation templating strategy to prepare two-dimensional carbon nanosheets with high nitrogen doping derived from petroleum asphalt, which were utilized as a versatile support for immobilizing Pd nanoparticles (Pd/N-CNS) in efficient Suzuki cross-coupling reactions. The results indicate that the anchoring effect of high-pyridinic N species on the two-dimensional carbon nanosheets enhances interactions between Pd and the support, effectively improving both the dispersibility and stability of the Pd nanoparticles. Notably, the Pd/N-CNS catalyst achieved an overall turnover frequency (TOF) of 2390 h−1for the Suzuki cross-coupling reaction under mild conditions, representing approximately a nine-fold increase in activity compared to commercial Pd/C catalysts. Furthermore, this catalyst maintained an overall TOF of 2294 h−1even after five reaction cycles, demonstrating excellent stability. Theoretical calculations corroborate these observed enhancements in catalytic performance by attributing them to improved electron transfer from Pd to the support facilitated by abundant pyridinic N species. This work provides valuable insights into feasible strategies for developing efficient catalysts aimed at sustainable production of biaromatic compounds.
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JOURNAL OF HAZARDOUS MATERIALS
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2024
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IF 12.2
Yongzhen Dong,Jiawei Liu,Liqin Kong,Dongyang Deng,Long Wu,Yiping Chen
This study presents the development of a magnetic relaxation switching (MRS) immunosensor for the sensitive detection of chlorpyrifos (CPF) with a signal amplification strategy using Pd/Cu-TCPP(Fe) hybrid nanosheets and polydopamine (PDA). Pd/Cu-TCPP(Fe) nanosheets, which exhibit high peroxidase-like activity and excellent storage stability, making them suitable replacements for natural enzymes in biosensors, are further functionalized with goat anti-mouse IgG (Ab 2 ) to construct an immunosensor. The mechanism relies on the competition between free CPF and the immobilized bovine serum albumin-CPF conjugates for antibody binding, which modulates the aggregation of magnetic nanoparticles (MNPs) that are related to the transverse relaxation time. The optimized immunosensor shows a linear detection range from 0.5 ng/mL to 100 ng/mL and a limit of detection (LOD) of 0.24 ng/mL, outperforming traditional enzyme-linked immunosorbent assay (ELISA) methods by achieving an LOD that is about 9 times lower. Real sample analysis demonstrates the applicability of the Pd/Cu-TCPP(Fe)-PDA-MRS immunosensor for detecting CPF residues in tomato and water samples, with results well consistent with those obtained using gas chromatography. This work highlights the potential of nanomaterials in enhancing the performance of MRS immunosensors for pesticide residue analysis in environmental and food safety monitoring.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2024
·
IF 3.8
Xuhai Zhu,Xiaobing Li,Rongjun Lin,Rui Lu,Fang Lu
Designing efficient catalysts for the preferential hydrogenation of vinyl groups is a pivotal challenge in the production of pharmaceuticals, agrochemicals, fine chemicals, dyes, and other valuable compounds. Herein, we developed evenly dispersed bimetallic Pd–Co nanoparticles on mesoporous silica nanospheres (MSNs) for selective hydrogenation of a model compound 3-nitrostyrene. By tuning the Pd/Co molar ratio and solvents, the efficiency of 3-nitrostyrene hydrogenation to 3-ethylnitrobenzene with the Pd1–Co1/MSN-Nb catalyst was well optimized; while 3-nitrostyrene was converted entirely, the selectivity of 3-ethylnitrobenzene was up to 95%. Moreover, this catalyst was stable and compatible with styrene and its derivatives. Further characterization results indicated that the combined effect of Pd-based metal nanoparticles and MSN-Nb and the electronic interaction between Pd and Co components in the Pd1–Co1/MSN-Nb catalyst have significant importance in the hydrogenation of 3-nitrostyrene. The aforementioned catalytic system will prove invaluable in guiding the selective hydrogenation of vinyl groups.
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