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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Materials
·
2024
·Vol. 17
·期 8
·1921
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IF 3.1
Yu Wang,Tao Xing,Lifeng Yan
Hydrogen is a dangerous gas as it reacts very easily with oxygen and may explode; therefore, the accumulation of hydrogen in confined spaces is a safety hazard. Composites consisting of unsaturated polymers and catalysts are a common getter, where the commonly used polymer is 1,4- diphenylethynyl benzene (DEB). Silicone rubber (SR) is a good carrier for hydrogen-absorbing materials due to its excellent chemical stability and gas permeability. In this work, polysiloxane, water, and a emulsifier are ultrasonically injected into a uniform emulsion, and the hydrogen getter DEB-Pd/C (Palladium on carbon) is then added. Under the catalysis of platinum (Pt), the cross-linking agent undergoes a hydrosilylation reaction to cross-link polysiloxane in emulsion to form silicone rubber. Then, the water was removed by freeze-drying, and the loss of water constructed a porous frame structure for silicone rubber, thus obtaining porous silicone rubber. The difference in hydrogen absorption performance between porous silicone rubber and ordinary silicone rubber was compared. It was found that, with the increase in water in the emulsion, the porous frame of silicone rubber was gradually improved, and the hydrogen absorption performance was improved by 243.4% at the highest, almost reaching the theoretical saturated hydrogen absorption capacity. Porous silicone rubber was prepared by emulsion mixing, which provided a new idea for further improving the hydrogen absorption performance of silicone rubber.
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Nature Communications
·
2024
·Vol. 15
·期 1
·1-18
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IF 14.7
Tang Xudong,Shang Yangyang,Yang Hong,Song Yalan,Li Shan,Qin Yusi,Song Jingyi,Chen Kang,Liu Yang,Zhang Dinglin,Chen Lei
The PD-1/PD-L1 pathway in mucosal immunity is currently actively explored and considered as a target for inflammatory bowel disease (IBD) treatment. However, systemic PD-L1 administration may cause unpredictable adverse effects due to immunosuppression. Here we show that reactive oxygen species (ROS)-responsive nanoparticles enhance the efficacy and safety of PD-L1 in a mouse colitis model. The nanoparticles control the accumulation and release of PD-L1 fused to Fc (PD-L1-Fc) at inflammatory sites in the colon. The nanotherapeutics shows superiority in alleviating inflammatory symptoms over systemic PD-L1-Fc administration and mitigates the adverse effects of PD-L1-Fc administration. The nanoparticles-formulated PD-L1-Fc affects production of proinflammatory and anti-inflammatory cytokines, attenuates the infiltration of macrophages, neutrophils, and dendritic cells, increases the frequencies of Treg, Th1 and Tfh cells, reshapes the gut microbiota composition; and increases short-chain fatty acid production. In summary, PD-L1-Fc-decorated nanoparticles may provide an effective and safe strategy for the targeted treatment of IBD.
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MOLECULAR CARCINOGENESIS
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2024
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IF 3
Qi Zhang,Chenying Yang,Zhijian Ma,Liangwen Ye,Yunfeng Wu,Caiyun Zhong,Ye Shi,Mingming Zhu
Sulforaphane (SFN) exerts anticancer effect on various cancers including gastric cancer. However, the regulatory effect of SFN on programmed death-ligand 1 (PD-L1) and checkpoint blockade therapy in gastric cancer have not been elucidated. Here we demonstrated that SFN suppressed gastric cancer cell growth both in vitro and in vivo study. SFN upregulated PD-L1 expression through activating ΔNP63α in gastric cancer cells. Further, we found that SFN impaired the anticancer effect of anti-PD-L1 monoclonal antibody (α-PD-L1 mab) on gastric cancer cells. These results uncover a novel PD-L1 regulatory mechanism and the double-edged role of SFN in gastric cancer intervention.
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ChemCatChem
·
2024
·
IF 3.8
Jinlian Liu,Liang Jiang,Bo Xing,Fuping Zhang,Yi Wang,Qilong Zhao,Mingliang Wu,Xin Chen,Guo Yang
Graphical The Pd/ZrO 2 catalyst prepared by the impregnation reduction method showed excellent activity and selectivity in the synthesis of HMTHF via the selective hydrogenation of the furan ring in 5-HMF at ambient hydrogen pressure and room temperature. Furthermore, the influence of the type of active hydrogen species on the hydrogenation of furan rings was proved by hydrogen spillover experiments. 5-Hydroxymethylfurfural (5-HMF) derived from lignocellulose represents an important platform molecule that could be employed in the selective hydrogenation of the furan ring to prepare 5‑hydroxymethyltetrahydrofurfural (HMTHF). However, the reported catalytic systems for the synthesis of HMTHF using 5-HMF still require additional hydrogen pressure. In this study, the Pd/ZrO 2 catalyst with uniformly dispersed Pd nanoparticles was prepared via a simple impregnation reduction process. This catalyst exhibited excellent catalytic activity and selectivity for the hydrogenation of 5-HMF to HMTHF. High HMTHF yields up to 92.3% were produced under mild reaction conditions of ambient hydrogen pressure and room temperature in methanol solvent. This result was superior to the most catalytic systems that had been reported so far. The mechanism study revealed that the active hydrogen species on the surface of the Pd nanoparticles and the reaction solvent in this study were the pivotal factors influencing the hydrogenation of furan rings in 5-HMF.
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CHEMICAL ENGINEERING JOURNAL
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2024
·
IF 13.3
Qinglei Wu,Chenyang Shen,Kaihang Sun,Menghui Liu,Chang-jun Liu
Tuning the hydrogenation activity of Pd is an effective method to achieve selective hydrogenation of acetylene. The previous study shows that Pd has a strong interaction with In 2 O 3 , causing a significant change in the electronic structure of the palladium catalyst. Herein, Pd/In 2 O 3 @SiO 2 was prepared by a deposition-precipitation method for selective hydrogenation of acetylene. After the reduction by flowing hydrogen, Pd-In intermetallic compounds can be formed. The concentration of the formed intermetallic compounds is closely associated with the reduction temperature. The Pd-In intermetallic compounds suppress the hydrogen activation ability of Pd and significantly weaken the adsorption of ethylene. Especially, a weak adsorption of di-σ-bonded ethylene is observed, which facilitates the desorption of ethylene and promotes the ethylene selectivity in the semi-hydrogenation of acetylene. The experimental study confirms that there exists an optimum reduction temperature (250 °C) for the formation of the Pd-In intermetallic compounds, with which ∼ 80 % ethylene selectivity and 100 % acetylene conversion have been achieved at 140 °C.
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JOURNAL OF CATALYSIS
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2024
·
IF 6.5
Qiang Zhou,Xinyu Wang,Tao Xing,Mingqing Wang,Mingbo Wu,Wenting Wu
Hydrogen peroxide (H 2 O 2 ) is widely used as an oxidant for photocatalytic oxidation of methane to value-added chemicals under mild conditions, but suffers from low utilization efficiency. Herein, we propose a comprehensive strategy for the proper amount of hydroxyl radicals (•OH) generation from H 2 O 2 by regulating the Pd/Au molar ratios and the total Au-Pd contents loaded on In 2 O 3 . For the photocatalytic oxidation of methane at ambient temperature, the yield and selectivity of CH 3 OH over the optimized 1.0% AuPd 0.5 /In 2 O 3 catalyst were as high as 2187.0 μmol g −1 h −1 and 94.0% respectively, exceeding most reported literatures. Mechanism investigations revealed that the formation of Au-Pd alloys may contribute to the homolytic cleavage of H 2 O 2 into •OH radicals and improve the selectivity of •OH generation. This work provides some guidance for the delicate design of photocatalysts to manipulate selective H 2 O 2 activation and efficient photocatalytic methane oxidation.
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MOLECULES
·
2024
·Vol. 29
·期 16
·3843
·
IF 4.2
Xinbao Li,Kai Sun,Ying Chen,Ye Yuan
As a widely used support, TiO2has often been combined with Pd to form highly sensitive gas-chromic materials. Herein, we prepared a series of Pd/TiO2catalysts with different Pd content (from 0.1 to 5 wt.%) by the impregnation method for their utilization in fast room-temperature CO detection. The detection was simply based on visible color change when the Pd/TiO2was exposed to CO. The sample with 1 wt.% Pd/TiO2presented an excellent CO gasochromic character, associated with a maximum chromatic aberration value of 90 before and after CO exposure. Systematic catalyst characterizations of XPS, FT-IR, CO-TPD, and N2adsorption–desorption and density functional theory calculations for the CO adsorption and charge transfer over the Pd and PdO surfaces were further carried out. It was found that the interaction between CO and the Pd surface was strong, associated with a large adsorption energy of −1.99 eV and charge transfer of 0.196e. The color change was caused by a reduction in Pd2+to metallic Pd0over the Pd/TiO2surface after CO exposure.
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CHEMICAL ENGINEERING SCIENCE
·
2025
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IF 4.3
Ruijie Ma,Huimin Gao,Jinpeng Zhang,Jieying Jing,Wen-Ying Li
Photocatalytic reduction of CO 2 to formic acid (HCOOH) offers a sustainable pathway for carbon utilization, yet its efficiency is fundamentally limited by poor CO 2 adsorption and rapid electron-hole recombination in conventional photocatalysts. To address this challenge, a series of Pd-loaded hydrogenated TiO 2 catalysts (x wt%Pd/H-TiO 2 ) were developed through a synergistic hydrogen reduction-impregnation strategy, aiming to regulate the electron density of Pd active sites and enhance interfacial charge separation. Systematic characterization revealed that increasing Pd loading (0.6–1.4 wt%) effectively trapped photogenerated electrons, suppressing recombination losses and elevating electron density at Pd sites. Combined with optimized CO 2 adsorption capacity (0.178 mmol·g −1 ) and accelerated charge transfer, the 1.0 wt%Pd/H-TiO 2 catalyst achieved a HCOOH production rate of 14.14 mmol·g cat −1 ·h −1 under mild conditions (30 °C, 2.0 MPa, 4.57 mW·cm −2 ), outperforming most reported TiO 2 -based systems. Mechanistic studies further demonstrated a strong correlation between Pd-induced electronic effects and multi-electron CO 2 activation kinetics. This work provides a scalable catalyst design paradigm for balancing charge dynamics and surface reactivity in photocatalytic CO 2 valorization.
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FOOD CHEMISTRY
·
2025
·
IF 9.8
Zhiwei Zhu,Shuqi Huang,Da-Wen Sun
The monitoring of ethylene continues to pose significant challenges for conventional sensors, primarily due to their instability when subjected to environmental fluctuations. Consequently, in the study, a coordination-stabilized Pd(II)/His@SiO 2 nanocomposite was engineered through the optimization of the histidine (His)-Pd(II) molar ratio (Pd-His-1-0.8). This was achieved by suppressing the hydrolysis/thermal decomposition of Pd(NO 3 ) 2 to ensure uniform dispersion of Pd(II) via His-SiO 2 hydrogen bonding. A 4 × 4 colourimetric sensor array, based on the Pd-His-1-0.8 and integrated with pH-responsive dyes, was constructed. This array generated unique fingerprints mediated by the Wacker reaction, facilitating the quantification of ethylene. The stability experiment proved that the sensor exhibited negligible signal drift across harsh conditions (25–70 °C, 43–81 % RH) and 21 d storage. Furthermore, some postharvest storage experiments using bananas as a representative fruit demonstrated that results obtained from the colourimetric sensor array were in good agreement with those from commercial detectors. This indicates the considerable potential of the sensors for applications in food and agricultural detection.
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JOURNAL OF POWER SOURCES
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2025
·
IF 7.9
Jinjuan Zhao,Sizhuo Ma,Aoxue Zhang,Yuner Xu,Zheng Liu,Mengjie Li,Honglei Yang,Ruifa Jin,Shuwen Li
The hydrogen-bonding interaction among catalytic center, support material and ethanol molecule can establish an effective microenvironment for ethanol oxidation reaction (EOR). However, the surrounding of palladium nanocrystals (Pd NCs) lacks highly electronegative atoms to form hydrogen bonds with ethanol molecule. To effectively address the limitation, suitable molecules can be incorporated into Pd-based catalysts alongside the selection of an appropriate support. The pyrene tetracarboxylate ionic liquid (PTCIL), composed of pyrene tetracarboxylate anions and quaternary ammonium cations, provides abundant oxygen atoms capable of forming hydrogen bonds with ethanol molecules and the oxygen-containing functional groups in reduced graphene oxide (RGO) support, thereby creating a conducive microenvironment towards green EOR. Additionally, PTCIL can be anchored onto the RGO support via π-π stacking, yielding abundant dispersed carboxyl and pyrenyl groups that act as active sites to stabilize Pd NCs. Furthermore, synergistic interactions within the catalyst enable electron transfer from PTCIL to Pd, weakening the adsorption strength of toxic intermediates. Herein, the prepared Pd/PTCIL-RGO-2 exhibits improved electrocatalytic activity (1523.2 mA mg −1 , 5.29 mA cm −2 ) compared to commercial Pd/C (807.2 mA mg −1 , 4.14 mA cm −2 ). This study proposes a design for constructing Pd-based catalysts with tailored local microenvironments, exhibiting enhanced activity and robust durability for versatile applications, including EOR and other small molecule oxidation reactions.
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Molecular Catalysis
·
2024
·
IF 3.9
Zhe Zhang,Jianan Zhang,Shuai Chen,Yanan Liu,Yufei He,Dianqing Li
Hydrogen spillover phenomenon can significantly impact the activity in hydrogenation reaction, but the spillover is limited in a very short range on non-reducible Al 2 O 3 , a most widely used industrial support. Herein, Al 2 O 3 doped with different lanthanides (ln) was prepared by co-precipitation, which was then used to produce Pd/ln-Al 2 O 3 catalysts. These catalysts display much higher hydrogenation activity towards alkylated anthraquinone than undoped Pd/Al 2 O 3 catalyst and those modified by non-lanthanide elements. After the introduction of lanthanides, the reaction order of H 2 decreases from 1 to 0. Further characterization and DFT calculation show that H 2 storage ability is increased for ln-doped catalysts due to the low activation energy of H transfer and low adsorption energy of H on O(-ln) sites. In addition, a reasonable relationship between reducibility of ln 3+ in catalysts and the catalytic performance is found.
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