CHEMICAL ENGINEERING JOURNAL
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2022
·
IF 16.744
Liuxuan Luo,Zehao Tan,Cehuang Fu,Rui Xue,Xiaojing Cheng,Tianzi Bi,Lutian Zhao,Yangge Guo,Xiyang Cai,Jiewei Yin,Shuiyun Shen,Junliang Zhang
Increasing the accessible active sites and especially improving the intrinsic activity are two major effective strategies for enhancing the electrocatalytic activity of nanomaterials. Accordingly, through the trioctylphosphine (TOP)-based CO-assisted solvothermal method and the small-amount Pt 2+ galvanic replacement, highly uniform Pd nanotetrahedrons (NTs) with Pt-doped surfaces are synthesized and supported onto carbon black. Comprehensive experimental and theoretical analyses reveal that, owing to the Pt surface-doped (SD) nanostructure, the conformal formation of surface Pt {111} facets, as well as the strain and electronic effects induced by the Pd–Pt alloy structure, Pd/ SD Pt NTs/C exhibits much better electrocatalytic performance than Pd NTs/C, commercial Pd/C, and Pt/C toward both oxygen reduction and formic acid oxidation reactions, showing greatly improved metal utilization and area/mass-specific activity. This study develops a high-performance bifunctional electrocatalyst, and firstly introduces TOP as the easy-removable surface-energy adjuster for the Pd shape-controlled synthesis, which may be further expanded to other metals and shapes.
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高影响因子
JOURNAL OF NANOBIOTECHNOLOGY
·
2022
·Vol. 20
·期 1
·1-17
·
IF 9.429
Lu Yuan-Fei,Zhou Jia-Ping,Zhou Qiao-Mei,Yang Xiao-Yan,Wang Xiao-Jie,Yu Jie-Ni,Zhang Jin-Guo,Du Yong-Zhong,Yu Ri-Sheng
Background The efficacy of immune checkpoint blockade (ICB), in the treatment of hepatocellular carcinoma (HCC), is limited due to low levels of tumor-infiltrating T lymphocytes and deficient checkpoint blockade in this immunologically "cool" tumor. Thus, combination approaches are needed to increase the response rates of ICB and induce synergistic antitumor immunity.Methods Herein, we designed a pH-sensitive multifunctional nanoplatform based on layered double hydroxides (LDHs) loaded with siRNA to block the intracellular immune checkpoint NR2F6, together with the asynchronous blockade surface receptor PD-L1 to induce strong synergistic antitumor immunity. Moreover, photothermal therapy (PTT) generated by LDHs after laser irradiation modified an immunologically “cold” microenvironment to potentiate Nr2f6-siRNA and anti-PD-L1 immunotherapy. Flow cytometry was performed to assess the immune responses initiated by the multifunctional nanoplatform.Results Under the slightly acidic tumor extracellular environment, PEG detached and the re-exposed positively charged LDHs enhanced tumor accumulation and cell uptake. The accumulated siRNA suppressed the signal of dual protumor activity in both immune and H22 tumor cells by silencing the NR2F6 gene, which further reduced the tumor burden and enhanced systemic antitumor immunity. The responses include enhanced tumor infiltration by CD4+ helper T cells, CD8+ cytotoxic T cells, and mature dendritic cells; the significantly decreased level of immune suppressed regulator T cells. The therapeutic responses were also attributed to the production of IL-2, IFN-γ, and TNF-α. The prepared nanoparticles also exhibited potential magnetic resonance imaging (MRI) ability, which could serve to guide synergistic immunotherapy treatment.Conclusion sIn summary, the three combinations of PTT, NR2F6 gene ablation and anti-PD-L1 can promote a synergistic immune response to inhibit the progression of primary HCC tumors and prevent metastasis. This study can be considered a proof-of-concept for the targeting of surface and intracellular immune checkpoints to supplement the existing HCC immunotherapy treatments.
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高影响因子
APPLIED CATALYSIS A-GENERAL
·
2022
·
IF 5.723
Longyu Xu,Shuya Hua,Jing Zhou,Yiqi Xu,Chunshan Lu,Feng Feng,Jia Zhao,Xiaoliang Xu,Qingtao Wang,Qunfeng Zhang,Xiaonian Li
Semi-hydrogenation of acetylene is one of the most promising methods to eliminate acetylene from ethylene / acetylene mixtures to avoid Ziegler−Natta polymerization catalysts being poisoned. Given that acetylene is always over-hydrogenated on conventional palladium-based catalyst, it is of great importance to facilitate the desorption of ethylene to enhance the ethylene selectivity. Herein, we report a simple method to anchor Pd by unsaturated penta-coordinated aluminum (Al 3+ penta ) on Al 2 O 3 (meso-Al 2 O 3 ). Characterized by 27 Al-NMR, XRD, HR-TEM, CO chemisorption and XPS, Pd/meso-Al 2 O 3 catalyst had a highly dispersion and unique electronic property of Pd, thus exhibiting a high ethylene selectivity (~83%) while the acetylene conversion is > 99%. Besides, the agglomeration of Pd is suppressed by the metal-support interaction (MSI) between Pd and meso-Al 2 O 3 support. Therefore, the preparation method of the catalyst is relatively simple and has certain commercial application prospects.
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MICROCHEMICAL JOURNAL
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2022
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IF 5.304
Jilan Qi,Xiaolei Zhang,Qiangyan Zhang,Ying Xue,Fei Meng,Yuanhua Liu,Gongjun Yang
In this work, a “signal on” electrochemiluminescence (ECL) strategy was proposed to detect Apolipoprotein-A1 (Apo-A1), a common tumor biomarker for bladder cancer. The tris(2,2′-bipyridyl)-ruthenium(II) [Ru(bpy) 3 2+ ] was used as luminophor captured by three-dimensional (3D) zinc oxalate metal–organic frameworks (MOFs), which constructed as the ECL nanoprobe (Ru-MOF) for detecting Apo-A1. Meanwhile, L-cysteine (L-Cys) as the co-reactant was connected to the [email protected] core–shell nanostructure through Au-S bond, which was directly modified on the glassy carbon electrode (GCE) to significantly reduce the electron transfer distance between the luminophor and co-reactant. The ECL intensity was “signal on” when the ECL probe of Ru-MOF was linked to the electrode by the immunoreaction of antigen–antibody. Based on these principles, the quantitative relationship between the concentration of Apo-A1 and the ECL intensity was obtained in the range of 1.00 fg·mL −1 to 1.00 ng·mL −1 with a linear coefficient of 0.9968. The proposed ECL immunosensor showed some great advantages, such as simplification, rapidity, stability and selectivity. It was also successfully applied for the determination of Apo-A1 in real serum and urine samples with the recovery of 98.0% ∼ 115.0% (RSD < 5.2%). To sum up, a “signal on” ECL immunosensor was successfully constructed for Apo-A1 detection, and it may facilitate the diagnosis of bladder cancer in clinic.
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Frontiers in Oncology
·
2022
·
IF 5.738
Da-Lai Xu,Yuan-Qing He,Bin Xiao,Yuan Si,Jian Shi,Xue-Ang Liu,Lei Tian,Qian Ren,Ya-Song Wu,Yi Zhu
Pancreatic ductal adenocarcinoma (PDAC) is a highly aggressive and lethal malignancy with a limited response to current therapies. Novel and effective treatment is urgently needed. Herein, a chimeric antigen receptor (CAR)-NK92 cell line, with an interleukin (IL)-15Rα-sushi/IL-15 complex and a Programmed cell death-1(PD1) signal inverter was constructed and named SP (
S
ushi-IL15-
P
D1). We showed that CAR expression enabled SP cells to proliferate independently of IL-2 and became more resistant to nutrition starvation-induced apoptosis. Meanwhile, SP cells were more effective than NK92 in PDAC cell killing assays in vitro and in vivo, and there was a positive correlation between the killing capability of SP cells and PD-L1 expression in pancreatic cancer cells. Based on the synergistic and comprehensive effects of the special CAR structure, the adhesion, responsiveness, degranulation efficiency, targeted delivery of cytotoxic granule content, and cytotoxicity of SP cells were significantly stronger than those of NK92. In conclusion, the SP cell line is a promising adoptive immunotherapy cell line and has potential value as an adjuvant treatment for pancreatic cancer, especially in patients with high PD-L1 expression.Keywords: pancreatic ductal adenocarcinoma, Chimeric antigen receptor (CAR), IL-15, IL-15Rα-sushi, programmed cell death ligand 1 (PD-L1), adoptive immunotherapy
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高影响因子
APPLIED ORGANOMETALLIC CHEMISTRY
·
2021
·Vol. 36
·期 3
·e6556
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IF 4.105
Wen-Jing Qiu,Ming-Wu Gao,Qi Chen,Ao Zheng,Yi-Jia Shi,Xin Liu,Juan-Hong Li,Guo-Liang Dai,Yang Hu,Zi-Xia Lin
Under normal temperature and pressure, a novel improved Fenton system that was named MHACF-MOF-808(Zr) was constructed after the introduction of Pd/MOF-808(Zr) and H 2 to solve the inherent problem of the production of iron sludge in the classic Fenton system. Only trace amount of Fe II was required during the whole reaction because Fe III could be rapidly reduced by the active hydrogen derived from the adsorption and activation of H 2 on the surface of Pd/MOF-808(Zr) composite. The concentration of Fe II could be maintained more than 10 μM. The removal of target pollutant sulfamethazine in this system was mainly relied on the degradation of ·OH verified by both of the direct detection and indirect inhibition (using methanol). By using the calculation of Laplacian bond order, the degradation pathway of sulfamethazine followed by the cleavage of N S bond. This prediction was verified by the detection of intermediate products. Only 21% sulfamethazine could be degraded after 3-h reaction in the classic Fenton reaction system, while it could be thoroughly degraded in 1.5 h in the MHACF-MOF-808(Zr) system. The influence of main parameters on the degradation effect of sulfamethazine, such as initial pH, the flow of H 2 , dosage of Pd/MOF-808(Zr), concentration of sulfamethazine, ferrous, and hydrogen peroxide, were systematically studied. Based on the relative stability of Pd/MOF-808(Zr) confirmed by the morphological characterization, sulfamethazine could be efficiently degraded in the MHACF-MOF-808(Zr) system.
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Molecular Catalysis
·
2023
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IF 4.6
Mengyu Dou,Yan Qiao,Xu Hu,Hengyang Miao,Ligong Zhou,Xuekuan Li,Xianglin Hou,Yingxiong Wang,Mingxing Tang
The poor textural properties of initial biochar materials have hindered their extensively applied as catalyst supports. Herein, cellulose biochar materials with the gradient porous and high specific surface area were synthesized by adding different ratios of ZnCl 2 , and as supports to prepare Pd/C cel catalysts for efficient maleic acid hydrogenation in water. The characterization results indicated that the textural propertiesand dispersion of Pd in Pd/C cel catalysts depended on the ratio of ZnCl 2 to cellulose. The Pd/C cel ZnCl 2(1:3) catalyst exhibited the best catalytic activity among all catalysts and outstanding stability for reusing 8 times under mild conditions (60 °C, 2 MPa). In addition, this synthesis strategy was also suitable for other biomass materials (glucose, sucrose, and starch) and the catalytic performance of ZnCl 2 -modified Pd/C catalysts in maleic acid hydrogenation reaction also improved dramatically. The carbonization mechanism was discussed by TG-MS and the results illustrated that ZnCl 2 reduced the carbonization temperature and altered the pyrolysis behavior of biochar as a result of excellent catalytic behavior. This work provided a facile and universal strategy for synthesizing biochar high-efficient supported catalysts with gradient porous structure and high specific surface area.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
·
IF 19.503
Shufang Ji,Yuanjun Chen,Guofeng Zhao,Yu Wang,Wenming Sun,Zedong Zhang,Yong Lu,Dingsheng Wang
Atomic-level insight into the unique catalytic capability of single-atom catalysts that distinguished from nanometer-sized counterparts is highly desirable for catalyst design and catalysis research. By synthesizing single Pd atoms supported on TiO 2 as a catalyst, here we demonstrate a steric hindrance effect of single atoms induced by the unique isolation of single-atom active sites to achieve a remarkable enhancement on catalytic performance in the synthesis of dimethyl carbonate. Experimental results and density functional theory calculations reveal that such steric hindrance effect of single atoms favors the yield of the desired product dimethyl carbonate against further reacting with intermediates to form byproduct, because no extra Pd species around single Pd atoms provide active sites to further adsorb and activate substrates directly. The discovery of such steric hindrance effect is a valuable supplement to single-atom catalysis, and may promote single-atom catalysts to be widely applied in selective catalytic reactions .
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CATALYSIS LETTERS
·
2021
·Vol. 152
·期 9
·2688-2694
·
IF 3.186
Cai Mingzhong,Liu Rong,Xu Caifeng,Huang Bin
Pd(OAc) 2 /XPhos–SO 3 Na in a mixture of poly(ethylene glycol) (PEG-400) and water is shown to be a highly efficient catalyst for the cyanation of aryl chlorides with potassium ferrocyanide. The reaction proceeded smoothly at 100 or 120 ºC with K 2 CO 3 or KOAc as base, delivering a variety of aromatic nitriles in good to excellent yields. The isolation of the crude products is facilely performed by extraction with cyclohexane and more importantly, both expensive Pd(OAc) 2 and XPhos–SO 3 Na in PEG-400/H 2 O system could be easily recycled and reused at least six times without any apparent loss of catalytic efficiency. Graphical Abstract Palladium-catalyzed cyanation of aryl chlorides with potassium ferrocyanide leading to aryl nitriles by using Pd(OAc) 2 /XPhos–SO 3 Na/PEG-400/H 2 O as a highly efficient and recyclable catalytic system is described.
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高影响因子
ANALYTICAL BIOCHEMISTRY
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2023
·
IF 2.9
Xuhuai Fu,Yunyao Lu,Yang Peng
Ultrasensitive detection of circulating tumor cells (CTCs) holds significant clinical importance in monitoring metastasis and therapeutic outcomes. In this study, we have developed a novel electrochemical sensing model based on nanomaterials for highly sensitive and specific determination of CTCs. A gold electrode co-modified with Ketjin black (KB) and Au nanoparticles (AuNPs) exhibits exceptional conductivity. By conjugating palladium-iridium cubic nanozyme (Pd–Ir CNE) with antibodies, we have created a detection probe capable of catalyzing hydrogen peroxide (H 2 O 2 ), thereby amplifying the output signal and resulting in significantly enhanced current on the electrode for detecting CTCs. The constructed immunosensor has achieved a detection limit of 2 cell mL −1 for model MCF-7 cells. Furthermore, the as-constructed electrochemical immunosensor can accurately detect whole blood-spiked target CTCs, showing great promise for clinical applications in early cancer diagnosis and prognosis.
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高影响因子
CRYSTENGCOMM
·
2023
·Vol. 25
·期 14
·2110-2118
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IF 3.1
Shi-Jun Yin,Li-Xian Li,Feng-Qing Yang
A polyhedral MIL-125-NH2@Pd nanoparticle with light-responsive oxidase-like activity was synthesized through a simple solvothermal method and was characterized by field emission scanning electron microscopy, transmission electron microscopy, energy-dispersive X-ray spectroscopy, X-ray powder diffraction, Fourier transform infrared spectroscopy, thermogravimetric analysis, Brunauer–Emmett–Teller analysis, etc. MIL-125-NH2@Pd can catalyze the oxidation of 3,3′,5,5′-tetramethylbenzidine (TMB) under light radiation without H2O2, indicating its intrinsic light-responsive oxidase-like characteristic. MIL-125-NH2@Pd shows a superior catalytic activity and higher affinity to TMB, compared to MIL-125-NH2, owing to the presence of homogenously distributed palladium (Pd) nanoparticles. The results of the mechanism study indicate the existence of ˙O2− and electron holes during the catalytic reaction of MIL-125-NH2@Pd. Furthermore, based on the excellent light-responsive oxidase-like activity and specific recognition capacity for casein phosphopeptides (CPP) of titanium ions (Ti4+) in MIL-125-NH2@Pd, a simple colorimetric sensing platform was developed for the determination of CPP in a linear range of 10–100 μg mL−1 with a limit of detection as low as 2.9 μg mL−1. Finally, the developed method was successfully employed in the sensitive and selective detection of CPP in spiked rabbit and rat plasma samples. This study may provide a reliable and highly efficient strategy to realize the excitation-responsive sensing applications of materials.
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NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 34
·16043-16049
·
IF 3.3
Hongbo Yu,Fei Zhang,Shuibo Wang,Yang Cong,Shiwei Wang,Lin Zhu
Hydrodeoxygenation of lignin-derived phenolic compounds to produce alkanes is a promising method used for mitigating fossil energy consumption, but they often require high temperature and high pressure, resulting in their poor catalytic stability and durability. In this study, we encapsulated ∼3.9 nm active metal Rh nanoparticles (NPs) into ∼40 nm hollow mesoporous aluminosilicate nanospheres (HMANs) to synthesize M@Alx–mSiO2 nanoreactors with adjustable Al contents for guaiacol hydrodeoxygenation. The optimized Rh@Al2.0–mSiO2 catalyst displayed significantly enhanced guaiacol activity and cyclohexane selectivity relative to the Rh@mSiO2 catalyst under mild reaction conditions. According to the characterization results, the high hydrodeoxygenation activity of Rh@Al2.0–mSiO2 could be attributable to the synergistic effect between the metallic Rh and Lewis and Brønsted acid sites, and the introduction of Al species greatly facilitated the adsorption of 2-methylcyclohexanol, thereby enhancing cyclohexane selectivity. The confinement effect of Rh NPs inside the hollow cavities effectively prevents the leaching and aggregation of Rh NPs, thereby improving their catalytic durability and stability.
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