LANGMUIR
·
2025
·
IF 3.9
Peng Guo,HongWei Li,BoYu Huang,Dong Ji,GuiXian Li,XinHong Zhao
Despite nitrogen-doped carbons (NC) enhancing metal–support interactions (MSI) in electrocatalysts, how specific N-configurations (pyridinic, pyrrolic, and graphitic) synergistically govern methanol oxidation reaction (MOR) pathways over Pd surfaces remains unknown. Herein, we hypothesize that precise thermal programming of ZIF-8 pyrolysis can tailor synergistic pyridinic-pyrrolic-graphitic N-triads to simultaneously enhance activity, CO tolerance, and stability. Guided by DFT predictions, Pd/NC-T catalysts (T = 700–1100) were synthesized, where in situ pyrolysis controls N-configurations (validated by XPS) and wet impregnation immobilizes ultrafine Pd nanoparticles (3.6 ± 0.8 nm). Furthermore, experimental and theoretical analyses reveal that pyrrolic-N facilitates the adsorption of methanol on Pd, while pyridinic-N suppresses the CHO* → CO* reaction pathway, thus enhancing the catalyst’s tolerance to poisoning, and graphitic-N prevents support dissolution and collapse during the electrocatalytic reaction, thus mitigating active site loss. Notably, Pd/NC-900 achieves 4195.0 mA·mg–1Pd in the alkaline electrolyte, maintaining 80.5% of its initial current density after 500 cycles at 200 mV/s, highlighting its exceptional catalytic activity and long-term stability. This work offers profound insights into the intricate MSI, serving as a crucial framework for guiding the future design and advancement of MOR electrocatalysts.
研究领域:
电化学
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催化
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材料科学
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纳米技术
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表面化学
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能量转换
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DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Haoqiang Feng,Yike Li,Xian Liu,Kang Wang,Qianhao Du,Yingju Wang,Zhongjun Li
Developing efficient piezo-photocatalysts through integrating cation vacancies with double metal single atoms is vitally important for hydrogen production, while it remains a challenge. In this work, cadmium vacancy (V Cd ) as well as Pt and Pd single atoms (Pt-Pd) were simultaneously introduced into CdS to construct V Cd -CdS/Pt-Pd catalysts for piezo-photocatalytic hydrogen evolution. In-depth characterizations and DFT calculations confirmed that the symmetry breaking caused by V Cd , Pt-Pd dual single atoms and ultrasonic could induce the polarization enhancement and charge asymmetric distribution, modulate the density of electronic states as well as optimize the adsorption of H* intermediates. Under light and ultrasound, the optimal V Cd -CdS/Pt 0.20 -Pd 0.30 achieved the piezo-photocatalytic hydrogen evolution rate of 104.4 mmol g −1 h −1 , which was 10.0 and 30.7 times that of V Cd -CdS and CdS, respectively. The significant improvement of piezo-photocatalytic performance was due to the synergistic interaction of V Cd -CdS, Pt-Pd double single atoms and the ultrasonic-induced external stress, which enhanced the polarized electric field in V Cd -CdS/Pt-Pd and promoted the separation and transfer of photo-generated charges. Moreover, the piezoelectric polarization induced by ultrasonic could tilt the energy band and produce a stronger reduction potential, also facilitating the hydrogen evolution reaction. On the whole, the symmetry breaking achieved by structure modifications coupled with external stress effectively boosted the piezo-photocatalytic hydrogen evolution performance, which provided a reference for the design of high-efficiency piezo-photocatalysts based on vacancy engineering and double single atoms doping.
研究领域:
材料科学
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催化
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可再生能源
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纳米技术
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物理化学
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产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Muchen Lu,Jie Sun,Boyang Cui,Jian Zhang,Junlian Ren,Ruoyi Li
In this study, Pd/Ru/MXene/ nickel foam (NF) electrodes were prepared by the impregnation method and galvanostatic electrodeposition technique to investigate their electrocatalytic degradation of tetracycline (TC). Subsequently, the electron transfer mechanism during this degradation process was studied. Under the optimal conditions, the degradation efficiency of the Pd/Ru/MXene/NF composite electrode for TC reached 92.02 % at 60 min. Bursting experiments as well as H 2 O 2 generation experiments showed that OH, H* and ClO − together realized the degradation of TC. The composite electrode could effectively reduce the biotoxicity of the intermediate products of the TC degradation process. In order to reduce the aggregation of Pd and Ru nanoparticles, a scaffold structure and the introduction of a MXene intermediate layer were used to solve the problem. Electrocatalytic degradation of antibiotic molecules was facilitated by tuning the interface of the catalytic electrode to expose active sites and modulating the electronic state of the catalyst to enhance intrinsic activity.
研究领域:
环境科学
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材料科学
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电化学
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DOI
高影响因子
Exploration
·
2025
·
IF 22.5
Qi Lu,Hao Ye,Jian Zhao,Xiaoyuan Fan,Kaiyuan Wang,Zeyu Han,Tian Liu,Lili Du,Jiaxuan Song,Helin Wang,Haotian Zhang,Zhonggui He,Jin Sun
The tumor microenvironment is characterized by immunosuppression and compromised intratumoral perfusion, which impairs the effectiveness of immune checkpoint inhibitors and nanomedicines. A significant challenge is the role of activated platelets, as they increase transfer-mediated PD-L1 expression from tumor cells and maintain the integrity of tumor vasculature. These platelets support tumor growth by stabilizing the vasculature and enabling immune evasion, as well as shielding tumor cells from immune detection. To address these platelet-mediated negative antitumor effects, we have developed bioengineered platelets (PTNPs) with surface-anchored ticagrelor-loaded gelatin nanoparticles. This study utilizes the natural tendency of platelets to localize their activated counterparts into tumors. Upon binding to tumor-associated activated platelets, the PTNPs release ticagrelor in response to the secreted matrix metalloproteinases by activated platelet, inhibiting further platelet activation. This reduction in platelet activation lessens platelet-facilitated immunosuppression and diminishes the transferred-PD-L1 expression from cancer cells to platelets, thus enhancing the immune response of anti-PD-L1 therapy. Additionally, this strategy weakens the activated platelets’ contribution to tumor vascular integrity, improving the extravasation and chemotherapeutic efficacy of nanomedicines. Our findings highlight the crucial role of platelet activation in tumor biology and introduce PTNPs as an effective approach to disrupt tumor-supporting platelet activities and enhance anticancer treatments efficacy.
研究领域:
肿瘤生物学
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免疫治疗
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纳米医学
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药理学
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生物材料
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产品关联
DOI
PubMed
高影响因子
Nature Communications
·
2022
·Vol. 13
·期 1
·1-17
·
IF 17.694
Guan Xin,Sun Liping,Shen Yuting,Jin Fengshan,Bo Xiaowan,Zhu Chunyan,Han Xiaoxia,Li Xiaolong,Chen Yu,Xu Huixiong,Yue Wenwen
Cancer recurrence after surgical resection (SR) is a considerable challenge, and the biological effect of SR on the tumor microenvironment (TME) that is pivotal in determining postsurgical treatment efficacy remains poorly understood. Here, with an experimental model, we demonstrate that the genomic landscape shaped by SR creates an immunosuppressive milieu characterized by hypoxia and high-influx of myeloid cells, fostering cancer progression and hindering PD-L1 blockade therapy. To address this issue, we engineer a radio-immunostimulant nanomedicine (IPI549@HMP) capable of targeting myeloid cells, and catalyzing endogenous H 2 O 2 into O 2 to achieve hypoxia-relieved radiotherapy (RT). The enhanced RT-mediated immunogenic effect results in postsurgical TME reprogramming and increased susceptibility to anti-PD-L1 therapy, which can suppress/eradicate locally residual and distant tumors, and elicits strong immune memory effects to resist tumor rechallenge. Our radioimmunotherapy points to a simple and effective therapeutic intervention against postsurgical cancer recurrence and metastasis.
研究领域:
肿瘤学
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免疫疗法
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纳米技术
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放射肿瘤学
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DOI
PubMed
高影响因子
PHYTOMEDICINE
·
2025
·
IF 8.3
Yufeng Deng,Qi hu,Zhiying Song,Mengyuan Nie,Zhiguo Wu,Yongrong Lei,Meng Liu,Dujuan Zhan,Baogang Xie
Objective Hepatocellular carcinoma (HCC) remains a leading cause of cancer mortality. Targeted therapies like lenvatinib face limitations due to resistance and immunosuppression. d -Glucaro-1,4-lactone (1,4-GL), a bioactive natural compound with anti-HCC activity, holds unexplored synergistic potential with lenvatinib. This study investigates the combinatorial efficacy of 1,4-GL and lenvatinib against HCC and elucidates the underlying mechanisms. Methods Efficacy was evaluated in H22 tumor-bearing mice treated with lenvatinib (20 mg/kg/day) ± 1,4-GL (25, 50, 100 mg/kg/day). Tumor inhibition, serum cytokines (TNF-α, IFN-γ, AFP), oxidative stress markers (MDA, SOD), liver enzymes (ALT, AST), and splenic T-cell subsets (flow cytometry) were assessed. Histopathology was analyzed via H&E staining. Lenvatinib pharmacokinetics (serum, liver, tumor) with/without 1,4-GL was determined in mice and SD rats using UPLC-MS/MS. In vitro, combinatorial effects on proliferation (CCK-8), migration (scratch assay), and clonogenicity (colony formation) were tested in Huh7 and HepG2 cells. STAT3 phosphorylation and PD-L1 expression (protein: Western blot; mRNA: RT-qPCR) were analyzed. PD-L1 induction was achieved using IFN-γ (20 ng/ml). Results The medium-dose combination (LMGL) achieved 89.97% tumor inhibition in H22 mice, significantly reducing tumor mass by 75% vs. lenvatinib alone (0.21±0.18 g vs. 0.84±0.79 g, p < 0.01). H&E staining revealed extensive necrosis in combination groups. Serum TNF-α and IFN-γ levels significantly increased ( p < 0.001), while AFP approached baseline. Flow cytometry showed an elevated CD4⁺/CD8⁺ T-cell ratio. Oxidative stress was modulated (reduced MDA and elevated SOD, p < 0.01). Pharmacokinetic studies revealed no significant differences in lenvatinib exposure or steady-state concentrations ( p > 0.05) with 1,4-GL co-administration. In vitro, 1,4-GL significantly reduced lenvatinib's IC 50 (Huh7: 18.54 μmol/l; HepG2: 30.34 μmol/l). Combinatorial treatment markedly downregulated PD-L1 protein/mRNA and inhibited STAT3 phosphorylation ( p < 0.05). Scratch and colony formation assays indicated synergy stemmed from immunomodulation and signaling inhibition, not enhanced anti-migration/proliferation. Conclusion 1,4-GL potently synergizes with lenvatinib against HCC by enhancing oxidative stress, reconstituting antitumor immunity, and suppressing the STAT3/PD-L1 signaling axis, without perturbing lenvatinib pharmacokinetics. This defines a novel phytochemical-based combinatorial strategy with significant clinical translation potential for HCC therapy.
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DOI
PubMed
高影响因子
INTERNATIONAL IMMUNOPHARMACOLOGY
·
2025
·
IF 4.7
Chunyu Qu,Hui Zhang,Minghao Sun,Siran Jin,Xiaodan Wu,Zhixiang Lan,Guanghui Tan,Zhiqiang Wang,Yujun Bao,Yingxue Jin
Immune checkpoint blockade (ICB) is a tumor therapy that leverages the activation mechanisms of T cells in the immune system. A key challenge in ICB is poor T-cell infiltration and low tumor immunogenicity. Immunogenic cell death (ICD) can increase tumor immunogenicity and make tumors more sensitive to ICB. Programmed death ligand 1 (PD-L1) a major target for ICB. In this paper, a novel carbon nitride/methyl pyrophaeophorbide a‑copper/folate (abbreviated as CNMCF) nanocomposite was prepared for induced ICD. In CNMCF nanostructures, methyl pyrophaeophorbide a (MPPa) serves as the photodynamic therapy (PDT) agent, and copper ion serves as the chemodynamic therapy (CDT) agent. CNMCF not only induced ICD, but also alleviated tumor hypoxia. This led to down-regulation of hypoxia-inducing factor (HIF-1 α ) and PD-L1, promoted T lymphocyte invasion, effectively enhanced tumor immunogenicity, and elicited strong anti-tumor immune response, thereby suppressing primary tumor growth and metastasis. This research expanded the application of natural chlorophyll derivatives and C 3 N 4 -based drug delivery systems in cancer immunotherapy.
研究领域:
生物医学工程
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免疫学
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肿瘤学
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产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2025
·
IF 4.3
Yaping Wang,Jie Liu,Chao Liu,Yongwei Lin,Xuefei Duan,Yongfei Ma,Hua Zhang,Muwen Deng,Qian Wang
The heterogeneity of tumors and complex pathways present significant challenges for effective treatment. In response, we developed a multifunctional platform combining photothermal therapy (PTT) and chemodynamic therapy (CDT), PB@Pd nanoparticles (NPs), to enhance the therapeutic efficacy of colorectal cancer. PB@Pd NPs were synthesized by doping palladium (Pd) on the surface of Prussian blue (PB) nanomaterials, enabling synergistic therapeutic effect. PTT generates localized hyperthermia, which accelerates the Fenton-like reaction and promotes the production of reactive oxygen species (ROS) in the tumor microenvironment. Meanwhile, ROS generated by CDT disrupts the tumor’s antioxidant defence system and increases the thermal sensitivity of cancer cells, thus enhancing the efficacy of PTT. This PTT/CDT synergistic approach overcomes the limitations of monotherapies, such as the limited penetration depth of PTT and the inefficiency of CDT in low H 2 O 2 environments. In vitro cellular experiments demonstrated that PB@Pd NPs significantly improved the therapeutic efficacy through synergistic effects. The nanoplatform also has good biocompatibility and stability, reducing the risk of side effects and drug resistance. By integrating PTT and CDT in vivo colon cancer model, PB@Pd NPs offer a promising strategy for more precise, efficient and less toxic tumor therapy, demonstrating their potential in advanced cancer therapies.
研究领域:
纳米医学
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肿瘤学
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光热治疗
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化学动力学治疗
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生物医学工程
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材料科学
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癌症治疗
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产品关联
DOI
高影响因子
JOURNAL OF NANOBIOTECHNOLOGY
·
2024
·Vol. 22
·期 1
·1-18
·
IF 10.6
Zou Ting,Huang Yun,Zhou Zongtao,He Shuangyan,Liu Jia,Chen Yalan,Liu Hongdu,Luo Zhonghui,Liu Miaoxin,Wei Hua,Yu CuiYun
Clinical treatment of hepatocellular carcinoma (HCC) with 5-fluorouracil (5-FU), the primary anticancer agent, remains unsatisfactory due to the glutathione (GSH)-associated drug resistance and immunosuppressive microenvironment of HCC. To develop a facile yet robust strategy to overcome 5-FU resistance for enhanced immunotherapy treatment of HCC via all dimensional GSH exhaustion, we report in this study construction of a minimalist prodrug consisting of 5-FU linked to an indoleamine-(2,3)-dioxygenase (IDO) inhibitor (IND) via a disulfide bridge, FU-SS-IND that can further self-assemble into stabilized nanoparticles, FU-SS-IND NPs. Specifically, besides the disulfide linker-induced GSH exhaustion, IND inhibits GSH biosynthesis and enhances the effector function of T cells for turning a “cold” tumor to a “hot” one, which synergistically achieving a tumor inhibition rate (TIR) of 92.5% in a 5-FU resistant mice model. Most importantly, FU-SS-IND NPs could upregulate programmed death ligand 1 (PD-L1) expression on the surface of tumor cells, which enables facile combination with immune checkpoint blockade (ICB) for a ultimate prolonged survival lifetime of 5-FU-resistant tumors-bearing mice. Overall, the minimalist bioreducible nano-prodrug developed herein demonstrates great translatable potential for efficiently reversing drug resistance and enhancing immunotherapy of HCC.
研究领域:
肿瘤学
·
药理学
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免疫疗法
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纳米医学
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产品关联
DOI
PubMed
高影响因子
BIOSENSORS & BIOELECTRONICS
·
2025
·
IF 10.5
Yingjing Fan,Weilun Pan,Qi Xiu,Yue Qiao,Peng Zhang,Tong Liao,Junjie Feng,Chengtao Nie,Shuai Chu,Ningcen Li,Xiuhua Wu,Lei Zheng,Zhen Cai,Bo Li
Tumor immunotherapy has significantly improved cancer treatment, yet immune checkpoint inhibitors only benefit a subset of patients. A critical challenge is non-invasive detection of tumor PD-L1 mRNA, a key biomarker that dynamically reflects PD-L1 expression and correlates with therapeutic outcomes. Current methods are hindered by the instability of circulating mRNA and the need for invasive tissue biopsies. Herein, we introduce the Cationic LIposome capsulated CRISPR-Cas13a Kit (CLICK) for in-situ detection of circulating PD-L1 mRNA in extracellular vesicles (EVs). CLICK achieves direct target identification in 10 μL plasma within 2 hours without EV purification or RNA extraction, demonstrating a detection limit of 10 3 EVs/mL for PD-L1 mRNA. By integrating membrane fusion-mediated CRISPR delivery with nanoflow cytometry, CLICK resolves PD-L1 mRNA (+) EV subpopulations at single-vesicle resolution, revealing heterogeneous distributions. Clinically validated in 53 immunotherapy patients, CLICK accurately stratifies progressive disease (PD) from stable disease (SD) patients (AUC = 0.8236; 95% CI: 0.7054–0.9417; p= 0.0006) based on PD-L1 mRNA (+) EV percentages. This work establishes a rapid, blood-based paradigm for therapy response monitoring, advancing liquid biopsy through precise EV RNA characterization.
研究领域:
肿瘤学
·
分子诊断
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转化医学
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免疫学
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RNA检测
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液体活检技术
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精准医学
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DOI
PubMed
高影响因子
JOURNAL OF LABELLED COMPOUNDS & RADIOPHARMACEUTICALS
·
2024
·Vol. 67
·期 11
·384-391
·
IF 0.9
Shuhua He,Lina Jia,Xiaobei Zheng,Yang Wang,Yuxia Liu,Lan Zhang
Programmed death-ligand 1 (PD-L1) expression is related to the efficacy and prognosis in triple-negative breast cancer. This study employed an indirect labeling method to synthesize [ 125 I]PI-Atezolizumab. The in vitro stability of [ 125 I]PI-Atezolizumab was assessed through incubation in phosphate buffered saline and fetal bovine serum, revealing sustained stability. Specific binding of [ 125 I]PI-Atezolizumab to MDA-MB-231 cells expressing humanized PD-L1 was assessed through in vitro incubation, yielding a K d value comparable to that of Atezolizumab. This suggests that the labeling process did not compromise the affinity of the Atezolizumab to PD-L1. Subsequently, pharmacokinetic studies were conducted in normal mice and biodistribution experiments in tumor-bearing mice. A comparison of the biodistribution results between [ 125 I]PI-Atezolizumab and 125 I-labeled Atezolizumab indicated better in vivo stability for the former. Single photon emission computed tomography (SPECT)/CT imaging further confirmed the targeted specificity of [ 125 I]PI-Atezolizumab for PD-L1 in MDA-MB-231 xenografts, which were validated by immunohistochemistry staining. This research underscores the utility of [ 125 I]PI-Atezolizumab, prepared via indirect labeling, for monitoring PD-L1 in triple-negative breast cancer models.
研究领域:
肿瘤学
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分子影像学
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放射性药物
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癌症生物学
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产品关联
DOI
PubMed
高影响因子
TETRAHEDRON
·
2024
·
IF 2.1
Zixu Li,Fei Wang,Kai Ma,Chao Fang,Qiang Jia,Changhu Chu
Aryl triflate is a type of facile and readily available compounds, which could be used as an alternative substrate for Suzuki cross coupling. In this manuscript, a novel ppm-Pd-Fe/C catalyst has been developed by reduction of palladium acetate and iron trichloride with aqueous hydrazine in situ and supported on activated charcoal. In combined with Sphos, and metal zinc as additives, this catalyst, with 300 ppm palladium loading, could be applied in the Suzuki cross coupling between aryl triflates with aryl neopentylglycolboronates.
研究领域:
有机化学
·
催化
·
材料科学
✓ 已验证
DOI
高影响因子