Catalysts
·
2016
·Vol. 6
·期 12
·181
·
IF 2.964
Jiahuan Yu,An Shen,Yucai Cao,Guanzhong Lu
A highly efficient and stable Pd-diimine@SBA-15 catalyst was successfully prepared by immobilizing Pd onto diimine-functionalized mesoporous silica SBA-15. With the help of diimine functional groups grafted onto the SBA-15, Pd could be anchored on a support with high dispersion. Pd-diimine@SBA-15 catalyst exhibited excellent catalytic performance for the Suzuki coupling reaction of electronically diverse aryl halides and phenylboronic acid under mild conditions with an ultralow amount of Pd (0.05 mol % Pd). When the catalyst amount was increased, it could catalyze the coupling reaction of chlorinated aromatics with phenylboronic acid. Compared with the catalytic performances of Pd/SBA-15 and Pd-diimine@SiO2catalysts, the Pd-diimine@SBA-15 catalyst exhibited higher hydrothermal stability and could be repeatedly used four times without a significant decrease of its catalytic activity.
研究领域:
催化化学
·
材料化学
·
有机合成
·
纳米材料
·
绿色化学
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
·
2024
·
IF 4.7
Xin-Hao Shen,Feng Liu,Qin-Qin Chen,Ying Gao,Xiao-Wen Wang,Xin Liu
The efficient degradation of emerging pollutants in water, represented by CBZ, is receiving increasing attention from all sectors of society. Although advanced oxidation reactions represented by Fenton reaction can efficiently degrade emerging pollutants, the problem of iron sludge that comes with it is hindering the further promotion of this technology. Herein, UiO-66(Zr)-2OH material was synthesized by hydrothermal method and loaded with Pd 0 NPs on the surface of the material by in situ reduction. The MOFs-H 2 -Accelerated Catalytic Fenton system was constructed by accelerating the regeneration of Fe(II) in the system by activating the [H] produced by H 2 introduced into the system at room temperature and pressure. Within 180 min, the removal of the target pollutant CZB could reach more than 99 % under the condition of only 25 µmol of Fe(II) and 25 mmol of H 2 O 2 .
研究领域:
环境科学
·
材料科学
·
化学工程
✓ 已验证
DOI
高影响因子
JOURNAL OF MEDICINAL CHEMISTRY
·
2024
·
IF 6.8
Zekun Zeng,Zhiwei Yang,Chenghao Li,Shujing Liu,Wei Wei,Ye Zhou,Simeng Wang,Mengjun Sui,Mengdan Li,Shumei Lin,Yangyang Cheng,Peng Hou
Despite the considerable achievements of antibodies targeting PD-1/PD-L1 in cancer immunotherapy, limitations in antitumor immune response and pharmacokinetics hinder their clinical adoption. Small molecules toward PD-L1 degradation signifies an innovative avenue to modulate PD-1/PD-L1 axis. Herein, we unveil a comprehensive engineering involving the development of new PD-L1 degraders based on the berberine (BBR) and palmatine (PMT) bioactive frameworks and explore their translational potential for cancer immunotherapy using a peptide-drug conjugate strategy. Chemical modifications at the O-9 position of PMT dramatically enhance the PD-L1 degradation capacity. Further conjugation of PMT degraders with an anti-PD-L1 peptide featuring disulfide linkers enables efficient GSH-specific prodrug activation, yielding synergistic immunotherapeutic benefits through both external PD-L1 blockade and internal PD-L1 degradation mechanisms. This work elucidates the compelling charm of the discovery and application of PD-L1 degraders, offering solutions to the challenges in advancing cancer immunotherapy in widespread clinics.
研究领域:
肿瘤学
·
免疫学
·
药学
·
分子生物学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
RSC Advances
·
2016
·Vol. 6
·期 106
·104398-104406
·
IF 3.289
Cong Zhang,Jingbo Qi,Jing Xing,Si-Fu Tang,Liang Song,Yuanyuan Sun,Chuanhui Zhang,Hongchuan Xin,Xuebing Li
Aqueous phase catalytic upgrading of lignin monomers to hydrocarbons via hydrodeoxygenation (HDO) has been explored using a combination of Pd/C and HZSM-5 catalysts under 2 MPa of H2 (ambient temperature). Model monomers with varying numbers of methoxy groups, including phenol, anisole, guaiacol and 2,6-dimethoxy-phenol, were chosen as lignin model compounds. Mechanistic studies revealed cascade and parallel reaction pathways via hydrogenation and dehydration (hydrolysis) processes, which were catalyzed by Pd/C and HZSM-5, respectively. Hydrogenation was preferred at lower temperature, whereas higher temperature was favorable for the removal of oxygen-containing functional groups. The effect of methoxy groups on the HDO of these monomers was also investigated systematically. Basically, the conversion of multi-substituted monomers was tougher than that of mono-substituted ones, due to steric constraint and the inhibition of the electron-donating hydroxyl group. The selectivities to cyclohexane from phenol and anisole were improved significantly by increasing the temperature to 413 K. However, cyclohexanone was preferably produced over cyclohexane when using model compounds with multi-substituents (guaiacol and 2,6-dimethoxy-phenol), even at temperatures above 513 K. Comparative experiments were also conducted on the HDO of 1,2-cyclohexanediol with or without the presence of phenol, which clearly suggested that the further HDO of guaiacol and 2,6-dimethoxy-phenol was inhibited, probably due to the strong interactions between cyclohexanediol molecules and Brønsted acid sites.
研究领域:
化学工程
·
催化反应
✓ 已验证
DOI
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
·
2020
·
IF 7.1
Tianjiao Meng,Huixian Jia,Siying An,Huan Wang,Xinjian Yang,Yufan Zhang
Herein, a Pd nanoparticles-DNA layered nanoreticulation (Pd NPs-DNA LNR) sensor was assembled to a graphene oxide (GO)-modified electrode by catalytic hairpin assembly (CHA) and a self-assembly process. In this process, GO was modified on the electrode surface to provide -COOH sites for DNA bonding. Moreover, with the CHA circular amplification strategy, many single DNA1 were exposed to be able to be bound with Pd-DNA2 for the formation of the Pd NPs-DNA LNR, which enabled the ultrasensitive detection of microRNA-21 (miR-21) with a low limit of detection 63.1 aM. This strategy combines the amplification technology of CHA and Pd NPs-DNA LNR with Pd NPs. Such a layered nanoreticulation material can support abundant Pd NPs to avoid aggregation and obtain enhanced electrochemical signals. Significantly, this method can be successfully applied in tumor cell lysates and provides a neoteric channel for early disease diagnosis.
研究领域:
生物传感器技术
·
分子诊断学
✓ 已验证
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2018
·
IF 6.434
Jiafeng Ding,Gaoyuan Long,Yang Luo,Runze Sun,Mengxia Chen,Yajun Li,Yanfang Zhou,Xinhua Xu,Weirong Zhao
Polychlorinated dibenzo- p -dioxins (PCDDs), as a group of notorious anthropogenic environmental toxicants, are arguably ubiquitous in nature. In this study, we investigated the photocatalytic reductive dechlorination of 2-chlorodibenzo- p -dioxin (2-CDD) over Pd/g-C 3 N 4 catalysts under UV–vis irradiation. The g-C 3 N 4 and a series of Pd/g-C 3 N 4 catalysts were prepared by thermal polymerization and mechanical mixing-illumination method and characterized by XRD, TEM, BET, SEM and UV–vis DRS analyses. Among all the samples, the Pd/g-C 3 N 4 (5 wt%) yielded the optimal dechlorination activity with a total 2-CDD conversion of 54% within 4 h, and 76% of those converted 2-CDD were evolved to dibenzo- p -dioxin (DD). The kinetics of dechlorination could be described as pseudo-first-order decay model (R 2 > 0.84). Corresponding rate constants (k) increased from 0.052 to 0.17 h −1 with Pd contents up to 5 wt% and decreased to 0.13 h −1 with a 10 wt% of Pd. The enhanced activities originated from the surface plasmonic resonance (SPR) effect of Pd nanoparticles and the formation of Schottky barrier between Pd and g-C 3 N 4 , which extend the spectrum responsive range and suppress the charge recombination of g-C 3 N 4 . This is the first report on the photocatalytic reductive removal of PCDDs and may provide a new approach for PCDDs pollution control.
研究领域:
环境科学
·
化学工程
✓ 已验证
DOI
高影响因子
Acta Pharmaceutica Sinica B
·
2025
·
IF 14.6
Yuhong Wang,Lin Hu,Lei Wang,Chonghai Zhang,Wenhao Shen,Hongli Yang,Min Li,Xin Zhang,Mengmeng Xu,Muxing Zhang,Kai Yang,Xiaopeng Tian
Inflammatory bowel disease (IBD) is an autoimmune disorder involving complex immune regulation, where balancing localized and systemic immunosuppression is a key challenge. This study aimed to enhance the therapeutic efficacy by engineering the probiotic Escherichia coli Nissle 1917 (EcN). We removed endogenous plasmids pMUT1 and pMUT2 from wild-type EcN and expressed the mPD-L1 (19‒238 aa)-mFc fusion protein on the bacterial surface using a cytolysin A (ClyA) fragment. This modification stabilized mPD-L1 (19‒238 aa) protein expression and promoted its recruitment to outer membrane vesicles (OMVs). The engineered strain, EcNΔ pMUT1/2 -ClyA-mPD-L1-mFc (EcN-ePD-L1-mFc), features conditional ePD-L1-mFc expression under the araBAD promoter, enhancing gut-targeted release and reducing systemic side effects. This strain improved treatment targeting and efficiency by enabling direct ePD-L1-mFc interaction with immune cells at inflammation sites. OMVs from this strain induced Treg proliferation, inhibited effector T cell proliferation in vitro , and significantly improved intestinal inflammation and colonic epithelial barrier repair in vivo . Additionally, the bacterium restored intestinal microbiota balance, increasing Lactobacillaceae and reducing Bacteroides . This study highlights the engineered bacterium's potential for targeted intestinal immune modulation and offers a novel local IBD treatment approach with promising clinical prospects.
研究领域:
微生物学
·
免疫学
·
分子生物学
·
胃肠病学
·
合成生物学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Molecular Catalysis
·
2025
·
IF 4.9
Lei Xia,Fang-Jing Liu,Meng-Jie Wang,Han-Bing Zhang,Jing Zhang,Yao Lu,Le-Le Qiu,Xian-Yong Wei,Yun-Peng Zhao
Production of cyclohexanone through selective hydrogenation of phenol under mild conditions has attracted much attention. Herein, a NaOH-modified Pd/WO 3 rich in oxygen vacancies for selective hydrogenation of phenol was prepared through impregnation method. The highest catalytic activity was exhibited on NaOH-Pd/WO 3 with 25 wt % addition of NaOH, and phenol achieved 100 % conversion at 90 °C and 0.7 MPa H 2 for 2 h, with a cyclohexanone selectivity of 95.3 %. The turnover frequency (TOF) of NaOH-Pd/WO 3 is approximately 3.5 times higher than that of the Pd/WO 3 . Detailed catalyst characterization and theoretical calculations reveal that the high activity and selectivity of NaOH-Pd/WO 3 for phenol hydrogenation to cyclohexanone are highly correlated with the concentration of oxygen vacancies in the catalyst. In-situ infrared and Raman analyses reveal that the OH - introduced by NaOH reacted with the lattice oxygen in WO 3 to abstract oxygen from the lattice, generating a significant number of oxygen vacancies. The possible reaction mechanisms for phenol hydrogenation were elucidated through combined density functional theory calculations and isotopic labeling experiments. This strategy of improving catalytic activity and selectivity by regulating the concentration of oxygen vacancies provides a theoretical basis for the design and optimization of industrial catalysts.
研究领域:
催化
·
化学工程
·
材料科学
·
物理化学
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2019
·
IF 4.084
Fufeng Cai,Peijing Lu,Jessica Juweriah Ibrahim,Yu Fu,Jun Zhang,Yuhan Sun
Methanol steam reforming is regarded as a very promising process to generate H 2 suitable for fuel cells. Typically, the Pd-based catalysts can catalyze efficiently methanol steam reforming for hydrogen production . But their high selectivity to CO, a byproduct of methanol reforming reaction , severely limits their potential application. In this work, a series of Nb-modified Pd−Zr−Zn catalysts with different Nb loadings were prepared to study their catalytic activities with more focus on the role of Nb on Pd−Zr−Zn catalyst for methanol steam reforming. The prepared catalysts were fully analyzed by using various characterization techniques, for example, ICP , BET, SEM, XRD , H 2 -TPR, NH 3 -TPD, HRTEM , CO chemisorption , XPS, and Raman. The experimental results showed that an increase in Nb loading for the Nb-modified Pd−Zr−Zn catalysts led to a decrease of the methanol conversion and H 2 production rate. This was probably due to the decrease in the amount of oxygen vacancies on the catalyst surface . However, introduction of Nb into Pd−Zr−Zn catalyst increased the acid strength on the catalytic surface. The aldehyde species derived from methanol decomposition were readily transformed to HCOOH, thus yielding high selectivity to CO 2 for the Nb-modified Pd−Zr−Zn catalysts. Significantly, the addition of Nb to Pd−Zr−Zn catalyst facilitated the incorporation of Pd into the ZnO lattices, which led to the formation of Pd−Zn alloy. Consequently, the Nb-modified Pd−Zr−Zn catalysts exhibited significantly lower CO selectivity and production rate than the Pd−Zr−Zn catalyst. From the results, this work offers a new way to the rational design of selective methanol steam reforming catalysts to decrease the formation of byproduct CO.
研究领域:
催化化学
·
能源材料科学
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2015
·
IF 3.313
Hansheng Wan,Qizhi Dong,Guiming Zhu,Gang Yu,Tianwu Yin,Meiling Huang
In this work, anatase-TiO 2 is investigated as a catalyst support in Pd/TiO 2 –C composite to improve the electrocatalytic properties of Pd for formic acid oxidation reaction (FAOR). Pd/TiO 2 has been synthesized by an impregnation-reduction method and then mixed with Vulcan XC-72R carbon black to obtain Pd/TiO 2 –C composite. Transmission electron microscopy (TEM) images show Pd nanoparticles (ca.3.5 nm in average diameter) in the Pd/TiO 2 –C (1:1) composite catalyst were dispersed on the surface of TiO 2 with a narrow particle size distribution . Electrochemical tests demonstrate Pd/TiO 2 –C (1:1) composite has significantly increased catalytic activity and stability compared with Pd/C for FAOR. The proposed reasons for these observations are the excellent acid corrosion and oxidation resistance of TiO 2 and the synergistic effect of Pd and TiO 2 nanoparticles . The effect of mass ratios of TiO 2 to C on the catalytic performance is also discussed. The best catalytic activity and stability for FAOR is found when the mass ratio of TiO 2 to C is 1:1. It can be interpreted as the synergistic effects and conductivity reach balance at this point.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
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.
研究领域:
催化化学
·
材料科学
·
有机合成
✓ 已验证
产品关联
DOI
高影响因子
ACS Catalysis
·
2022
·
IF 13.7
Xin Song,Fangjun Shao,Zijiang Zhao,Xiaonian Li,Zhongzhe Wei,Jianguo Wang
It is challenging to develop an alkyne semi-hydrogenation catalyst with both high selectivity and high activity, especially at low temperatures and low pressures. Herein, a single-atom Ni-modified Al2O3-supported Pd is proposed as a modulation strategy to optimize the selectivity of alkyne semi-hydrogenation. Sphere-difference-corrected transmission electron microscopy and synchrotron radiation confirm that Ni single atoms enter the alumina lattice in a highly dispersed state, while Pd is loaded on the Ni-modified support in the form of nanoparticles. For the semi-hydrogenation of phenylacetylene, the Pd0.5/Ni0.5@γ-Al2O3 catalyst with Pd and Ni loadings of 0.45 and 0.43 wt %, respectively, achieves 98% conversion and 94% selectivity at 298 K and 0.1 MPa. It also possesses good stability, as the activity remains unchanged after 10 cycles of application. The Pd0.5/Ni0.5@γ-Al2O3 catalyst inherits the high activity of Pd and the high selectivity of Ni to achieve efficient semi-hydrogenation of phenylacetylene at low temperatures and pressures, benefiting from the synergistic effect of Pd and Ni.
研究领域:
催化
·
材料科学
·
化学工程
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）