International Journal of Electrochemical Science
·
2023
·Vol. 7
·期 1
·106-119
·
IF 1.5
Yun Zhi Fu,Yun Yang
Nanostructured Pd networks were synthesized in high yield through the reduction of Pd (acac) 2 using oleylamine as the solvent, reductant and capping agent. The formation of the network Pd nanostructure is due to oriented attachment among the formed primary particles at high temperature. By adjusting the reaction time, concentration of Pd precursor and reaction temperature, their thickness and interconnectivity can be tuned. The prepared nanostructured Pd networks exhibit efficient electrocatalytic activities toward the oxidation of formic acid in acid media. The enhanced electrocatalytic properties of Pd networks can be attributed to the interconnectivity and presence of a large number of active sites on their surfaces.
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Scientific Reports
·
2026
·
IF 4.9
Zhou Kun,Yuan Wei,Zhang Fan
Radix Bupleuri-Radix Paeoniae Alba (RB-RPA) has the potential to ameliorate the immune microenvironment in hepatocellular carcinoma (HCC). The interactions between various cells influence the immune microenvironment. However, the effects of the active components (saikosaponin D (SSD) and paeoniflorin) of RB-RPA on HCC and the cell interactions within its microenvironment warrant further investigations. We established orthotopic mouse models of HCC using Hepa 1–6 cells (a hepatoma cell line) to investigate the infiltration of cancer-associated fibroblasts (CAFs). Following this, we knocked down CLCF1 in the CAFs to explore their interactions with Hepa 1–6 cells. We subsequently treated CAFs with SSD-paeoniflorin. In T-cell activation assays, we overexpressed PD-L1 in Hepa 1–6 cells and co-cultured these cells with T cells. Additionally, we treated HCC mice with SSD-paeoniflorin and induced the overexpression of CLCF1 in vivo. In mice with HCC, tumors were characterized by substantial infiltration of CAFs, which displayed elevated levels of the protein CLCF1. These CAFs play a role in suppressing the HCC immune microenvironment and elevating PD-L1 levels through the production of CLCF1. At the cellular level, SSD-paeoniflorin inhibited the growth of CAFs and the expression of CLCF1 and also suppressed the PD-L1 level in Hepa 1–6 cells through CAF-derived CLCF1. Mechanistically, CLCF1 may promote PD-L1 expression via the JAK/STAT3 signaling pathway. Furthermore, the overexpression of PD-L1 in Hepa 1–6 cells suppressed T cell proliferation and activation. In animal studies, SSD-paeoniflorin improved the HCC immune microenvironment by enhancing the interaction between CAFs and Hepa 1–6 cells through CLCF1. Collectively, SSD-paeoniflorin inhibits CLCF1 secretion in CAFs to downregulate PD-L1 expression in Hepa 1–6 cells and may reactivate the anti-tumor immune microenvironment in HCC.
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ChemNanoMat
·
2023
·Vol. 9
·期 5
·e202200569
·
IF 3.8
Yanyu Li,Xiaoyue Zhang,Jinglin Shen,Wei Qi
Graphical A new type of nanocomposite enzymes has been developed, composed of Pd−Pt nanoparticles, hemin-rGO and CNTs-COOH. The nanocomposites show a high peroxidase-like activity and a linear response toward H 2 O 2 in the range of 0.05–500 μM with a determination limit of 0.01 μM. Based on this, a paper sensor was constructed for H 2 O 2 detection in real samples. Nanocomposite enzymes are attracting intensive attention worldwide. In the present study, a novel colorimetric H 2 O 2 paper sensor was developed based on a new type of nanocomposites composed of Pd−Pt nanoparticles, hemin functionalized reduced graphene oxide (hemin-rGO) and carboxylated carbon nanotubes (CNTs-COOH). The proposed nanocomposites show a high peroxidase-like activity. It provides a sensitive platform showing a linear response toward H 2 O 2 in the range of 0.05–500 μM with a determination limit of 0.01 μM. Based on this, the composites were applied to construct a paper sensor for H 2 O 2 detection in real samples. The cost-effectiveness, simplicity and efficiency of this paper sensor could be developed for “point-of-care” analysis and other related areas.
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Acta Biomaterialia
·
2023
·
IF 9.7
Bo Li,Tong Yang,Jin Liu,Xixi Yu,Xinying Li,Fei Qin,Jiefei Zheng,Jinxia Liang,Youyan Zeng,Zhenhua Zhou,Lu Liu,Bin Zhang,Weiwei Yao,Zhuo Feng,Guandi Zeng,Qian Zhou,Liang Chen
Non-small cell lung cancer (NSCLC) remains the most frequently diagnosed lung cancer and the leading cause of cancer-related mortality worldwide. PD-1/PD-L1 axis inhibitors have changed the treatment paradigm for various cancer types, including NSCLC. However, success of these inhibitors in lung cancer clinic is severely limited by their inability to inhibit the PD-1/PD-L1 signaling axis due to heavy glycosylation and heterogeneity expression of PD-L1 in NSCLC tumor tissue. Taking advantage of the facts that tumor cell derived nanovesicles could efficiently accumulate in the homotypic tumor sites due to their innate targeting abilities and that specific and high affinity existed between PD-1 and PD-L1, we developed NSCLC targeting biomimetic nanovesicles (NV) cargos from genetically engineered NSCLC cell lines that overexpressed PD-1 (P-NV). We showed that P-NVs efficiently bound NSCLC cells in vitro and targeted tumor nodules in vivo . We further loaded P-NVs with 2-deoxy-D-glucose (2-DG) and doxorubicin (DOX), and found that these drugs co-loaded P-NVs efficiently shrank lung cancers in mouse models for both allograft and autochthonous tumor. Mechanistically, drug-loaded P-NVs efficiently caused cytotoxicity to tumor cells and simultaneously activated anti-tumor immunity function of tumor-infiltrating T cells. Our data therefore strongly argue that 2-DG and DOX co-loaded, PD-1-displaying nanovesicles is a highly promising therapy for treatment of NSCLC in clinic. Statement of significance Lung cancer cells overexpressing PD-1 are developed for preparing nanoparticles (P-NV). PD-1s displayed on NVs enhance their homologous targeting abilities to tumor cells expressing PD-L1s. Chemotherapeutics such as DOX and 2-DG, are packaged in such nanovesicles (PDG-NV). These nanovesicles efficiently delivered chemotherapeutics to tumor nodules specifically. The synergy between DOX and 2-DG is observed in inhibiting lung cancer cells in vitro and in vivo . Importantly, 2-DG causes deglycosylation and downregulation of PD-L1 on tumor cells while PD-1 displayed on nanovesicles’ membrane blocks PD-L1 on tumor cells. 2-DG loaded nanoparticles thus activate anti-tumor activities of T cells in the tumor microenvironment. Our work thus highlights the promising antitumor activity of PDG-NVs, which warrants further clinical evaluation.
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高影响因子
MATERIALS CHEMISTRY AND PHYSICS
·
2023
·
IF 4.6
Xiao Teng,Bo Zhang,Luxia Yin,Wanyi Tao,Zhang Wen,Zekai Zhang,Wensheng Ning
A series of PdO/CeO 2 /SiO 2 -z aerogel composites with different molar ratio of Si/Ce were facilely fabricated via sol-gel method combined with atmospheric drying technology, where a major of Ce 3+ species could be oxidized to Ce 4+ species by adding hydrogen peroxide. They were used to remove thiophenics from model fuels and aromatics, compared with PdO/SiO 2 and CeO 2 /SiO 2 aerogel composites. Adding Ce and Pd led to an appearance of weak Lewis acid centers on the surface of adsorbents. Compared with PdO/SiO 2 and CeO 2 /SiO 2 , the adsorption capacity of PdO/CeO 2 /SiO 2 -z significantly increased, in which PdO/CeO 2 /SiO 2 -100 performed best and the adsorption capacity for thiophene was 15.0 mg-S/g ads , which was about the sum of PdO/SiO 2 -636 and CeO 2 /SiO 2 -100. The case was attributed to π-complexation of Pd 2+ and S-M (Pd, Ce, acted as Lewis acid centers) bond (σ) with thiophenics, where the adsorption process was dominated by S–Ce bond. Combined with the same chemical state of Pd and Ce in single metal and bimetal adsorbents verified by XPS , it can be deduced that no synergistic interaction between Pd and Ce species was formed in the adsorption process. PdO/CeO 2 /SiO 2 -100 exhibited a higher resistance for competitive adsorption of aromatics and a good solvent washing regeneration performance. The adsorption process of PdO/CeO 2 /SiO 2 -100 for thiophene was well fitted by Langmuir isothermal and pseudo-secound-order model and were spontaneous and endothermic. The solvents (n-heptane, benzene and p-xylene) have no obvious effect on the adsorption thermodynamics and kinetics of PdO/CeO 2 /SiO 2 -100.
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Small Structures
·
2023
·Vol. 4
·期 10
·2300137
·
IF 15.9
Jingpeng Li,Rumin Ma,Sisi Yao,Daochun Qin,Yun Lu,Yuhe Chen,Zehui Jiang,Dongjiang Yang
Plant-based flow microreactors with natural channel structures, renewable properties, and environmental friendliness have increasingly gained popularity in heterogeneous catalysis. However, firmly immobilizing the catalysts simultaneously with ease and adaptability, maintaining great effectivity and long-term stability, is still a fundamental challenge. Herein, a highly efficient and ultrastable bamboo-based catalytic microreactor (CMR) containing mesoporous TiO 2 (M-TiO 2 )-encapsulating ultrafine Pd nanoparticles (NPs) is constructed for the continuous-flow hydrogenation of nitroaromatics. The fabrication of the Pd-TiO 2 catalysts in required bamboo microchannels (Pd-TiO 2 /B CMR) mainly involves a two-step region-selective synthetic strategy with ultra-low chemical usage, fast preparation, and low catalyst loading (0.007 wt%). The M-TiO 2 films: 1) provide abundant oxygen vacancies and enough open cavities to facilitate the growth of Pd NPs; 2) improve Pd dispersion and reduce particle size; 3) allow diffusion of reactants, and 4) induce strong metal-support interactions for enhanced catalytic activity and stability. The optimized Pd-TiO 2 /B CMR demonstrates high efficiency (>97%) and excellent stability (1,000 h) for the continuous-flow hydrogenation of nitroaniline, even under intermittent operation (12 h on/12 h off for five cycles) or in a real aqueous matrix (>200 h), making it a promising candidate for Pd-catalyzed hydrogenation.
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ACS ES&T Engineering
·
2023
·
IF 7.1
Jia Xie,Zhengjun Lv,Linhan Ni,Hao Zhang,Xin Yan,Yujun Zhou,Zhigao Zhu,Junwen Qi,Xiuyun Sun,Jiansheng Li
Rapid and economic removal of N-nitrosodimethylamine (NDMA) calls for advanced treatment strategies due to its mutagenic and carcinogenic effects, small molecular size, high polarity, and uncharged properties. Herein, a sequential Pd-modified polymeric ultrafiltration (UF) membrane coated on a carbon paper substrate (CpPdM) was designed for the complete elimination of NMDA in one single pass with low energy consumption, with the synergetic processes of direct electrochemical reduction and Pd-catalyzed hydrogenation. The hydrogen gas, produced from direct electrochemical reduction, could trigger the Pd-catalyzed hydrogeneration to improve the NDMA destruction performance. In addition, the pre-rejection of interfering substances in the water matrix by the frontmost UF layer hugely mitigates the fouling issues on the electrode, thus improving the stability. Moreover, the flow-through operation mode overcame the mass transfer limitation of traditional electrodes in the flow-by mode (100% NDMA removal within 12.6 s of residence time at −2.3 V), resulting in 2 orders of magnitude enhancement in modified reaction kinetics. Furthermore, the combined treatment of the CpPdM and nanofiltration was superior to the conventional reverse osmosis process in NDMA removal and energy use. This work is expected to provide a new strategy for developing an energy-efficient advanced wastewater treatment system.
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Sustainable Energy & Fuels
·
2023
·Vol. 7
·期 13
·3096-3105
·
IF 5.6
Zhongxuan Lin,Ouyang Liu,Shuyan Guan,Xinru Zhao,Zhenluo Yuan,Xianyun Liu,Linyan Bian,Yanping Fan,Qiuming Peng,Shumin Han,Baozhong Liu
An efficient and promising liquid chemical substance for hydrogen storage and production at room temperature is formic acid (FA). In this study, a series of N-doped carbon dot supported Pd nanoparticles (NPs) with mean particle sizes ranging from 1.94 to 2.65 nm were produced and utilized to catalyze efficient dehydrogenation from FA aqueous solution at ambient temperature. The Pd/CD catalysts demonstrated exceptional catalytic performance in FA dehydrogenation without producing CO, resulting in the production of hydrogen. The Pd/CDs-III catalyst delivered 100% FA dehydrogenation in 21 minutes and a TOF value of 256 h−1 at 298 K. Furthermore, electron-rich Pd played a crucial role in facilitating the rupture of the C–H bond. Additionally, the combination of N and self-crosslinked carbon dots assisted in controlling the growth of Pd NPs and improving their dispersion, inhibiting aggregation during the reaction test. This work offers valuable insights for the synthesis of N-doped carbon dot supported highly dispersed Pd-based catalysts for FA dehydrogenation in water.
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Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Xiaoyu Zhong,Linyang Li,Wenhao Xiang,Chuanbao Xiao,Nianbing Zhong,Quanhua Xie,Dengjie Zhong,Yunlan Xu,Haixing Chang,Shih-Hsin Ho
Herein, a highly stable and efficient photoelectrocatalytic system was developed for the rapid degradation of tetracycline . The photoelectrocatalytic system comprised two Ag/N-doped TiO 2 nanotube photoanodes, a bipolar membrane, and a P–Pd cathode. The Ag/N-doped TiO 2 nanotube photoanodes were coupled with a P–Pd cathode to enhance the hydroxyl free radical (·OH) generation at the cathode surface. The bipolar membrane can separate tetracycline pollutants and degradation products from the photoanodes, which can minimize the contamination of the photocatalyst by tetracycline or products, thereby enhancing the repeatability and stability of the photoelectrocatalytic system. photoelectrocatalytic uses ultraviolet–visible light as the input energy for the effective removal of tetracycline and total organic carbon . The initial pH in the cathode and photoanode chambers was 7.0. The Na 2 SO 4 concentration in the photoanode chamber and the addition amount of H 2 O 2 were 0.2 M and 4% (v/v), respectively. Under these conditions, 100 mL of 100 mg/L tetracycline was completely degraded within 60 min, and 82.3% total organic carbon was removed within 5 h. The pseudo-first-order reaction rate constant of the Ag/N-doped TiO 2 nanotube with 0.15 M Ag was 0.0637 min-1, which was 12 times higher than that of N-doped TiO 2 nanotube. The mechanisms underlying·OH generation and the tetracycline degradation pathway were also elucidated. The photoelectrocatalytic system, which is an eco-friendly and low-energy system, exhibits excellent stability and reliability toward tetracycline and total organic carbon degradation and significantly aids the development of wastewater remediation.
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CHEMOSPHERE
·
2023
·
IF 8.8
Guobo Li,Yaping Zhang,Peng Wu,Kai Shen,Shule Zhang,Shipeng Ding
The synergistic degradation of VOCs and NO x that were emitted from the incineration of municipal and medical wastes by a single catalyst is challenging, due to the poor activity at low temperatures, and the SO 2 poisoning on the active sites. Herein, N-doped TiO 2 (N–TiO 2 ) was used as the support for designing a highly efficient and stable catalyst system for CB/NO x synergistic degradation even in the presence of SO 2 . The prepared SbPdV/N–TiO 2 catalyst, which presented excellent activity and tolerance to SO 2 in the CBCO + SCR process, was investigated by a series of characterizations (such as XRD, TPD, XPS, H 2 -TPR and so on) as well as DFT calculations . The electronic structure of the catalyst was effectively modulated after N doping, resulting in effective charge flow between the catalyst surface and gas molecules. More importantly, the adsorption and deposition of sulfur species and reaction transient intermediates on active centers were restrained, while a new N adsorption center for NO x was provided. Abundant adsorption centers and superior redox properties ensured smooth CB/NO x synergistic degradation. The removal of CB mainly follows the L-H mechanism, while NO x elimination follows both E-R and L-H mechanisms. As a result, N doping provides a new approach to develop more advanced anti-SO 2 poisoning CB/NO x synergistic catalytic removal systems for extensive applications.
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高影响因子
MOLECULES
·
2023
·Vol. 28
·期 3
·922
·
IF 4.6
Pengcheng Li,Jingjing Zhu,Hongyu Zhang,Lan Wang,Shulin Wang,Mengting Zhang,Jianping Wu,Lirong Yang,Gang Xu
Chiral amines are essential components for many pharmaceuticals and agrochemicals. However, the difficulty in obtaining enantiomerically pure amines limits their application. In this study, hollow amorphous ZIF-90 (HamZIF-90) materials were prepared by template engraving, and chemical–enzyme coupling catalysts (HamZIF-90@Pd@CALB) were constructed for the chiral resolution of 1-phenylethylamine. Different from conventional materials, HamZIF-90 had tunable hollow structures by altering its central node zinc ion concentrations, and the embedded hydrogel template gave it more pore structures, which facilitated the loading of enzyme molecules and Pd nanoparticles (NPs). The establishment of the coupling catalysts shortened the mass transfer distance of the reactant molecules between the metal nanoparticles and the enzyme catalyst in the dynamic kinetic resolution (DKR) reaction, resulting in 98% conversion of 1-phenylethylamine and 93% selectivity of Sel.R-amide. The proposal of this idea provided a good idea for future tailor-made MOFs loaded with chemical and enzyme coupled catalyst.Keywords:hollow amorphous;HamZIF-90@Pd@CALB;DKR;1-phenylethylamine
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高影响因子
CHEMOSPHERE
·
2023
·
IF 8.8
Sini Lv,Fengzhen Zheng,Zeyu Wang,Luyao Dai,Huan Liu,Dzmitry Hrynshpan,Tatsiana Savitskaya,Jun Chen
The high hydrophobicity of n -hexane is the main reason why it is difficult to be removed biologically. In this study, the effects of bamboo-charcoal modified by bimetallic Fe/Pd (BBC) on n -hexane biodegradation by Pseudomonas mendocina NX-1 (PM) was investigated. The n- hexane removal efficiency was increased in the presence of BC. The highest n- hexane removal efficiency at 90.0% was achieved at 0.05 g L −1 BCE and 3 g L −1 NH 4 + under pH 7.7 and 35 °C. Additionally, protein content (45.9 μg mL −1 ) and negative cell surface zeta potential (−26.4 mV) were increased during biodegradation process, with PM-BBC being 43.1 μg mL −1 and 19.1 mV. Bacterial growth was improved and maximum cell surface hydrophobicity was obtained after 20 h, which was 59.4% higher than the control with PM-BBC (37.7%) or PM (16.1%), showing biodegradation products of 1-butanol and acetic acid. The results indicate that BBC improved n- hexane biodegradation efficiency by promoting bacterial growth, reducing cell zeta potential, exposing hydrophobic proteins, and increasing cell surface hydrophobicity of bacterial strain NX-1. This investigation suggests that BBC-enhanced biodegradation can be promising to treat n- hexane-containing gas.
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高影响因子
危险品化学品经营许可证（带存储）