JOURNAL OF CATALYSIS
·
2018
·
IF 6.759
Renshan Wang,Benxia Li,Yi Xiao,Xueqin Tao,Xintai Su,Xiaoping Dong
Ultrathin semiconductor nanosheets decorated with metallic nanoparticles (NPs) are promising in photocatalysis due to the multi-component interactions. The materials with a series of monometallic Pd and bimetallic Au-Pd NPs anchored on Bi 2 WO 6 ultrathin nanosheets were synthesized and developed as photocatalysts for selective oxidation of aromatic alcohols to aromatic aldehyde. By optimizing the metallic contents, a typical sample of Au(0.25)Pd(0.25)-Bi 2 WO 6 exhibited the highest photocatalytic activity among all the prepared photocatalysts including Au(0.5)-Bi 2 WO 6 , Pd( x )-Bi 2 WO 6 , Au( x )Pd( x )-Bi 2 WO 6 ( x represents the weight percentage of metal in the photocatalyst), along with the improved selectivity for producing benzaldehyde. The extended absorption in visible range, higher efficiency for the transfer and separation of photogenerated charge carriers, and the superior ability for generating active radicals of Au(0.25)Pd(0.25)-Bi 2 WO 6 were demonstrated by DRS spectra, photoelectrochemical measurements, and ESR detection. The effect of the active species for selective oxidation of aromatic alcohols was proved to follow the order of h + + O 2 − > h + >> O 2 − . Accordingly, a possible mechanism based on the interfacial cooperation between bimetallic Au-Pd NPs and Bi 2 WO 6 ultrathin nanosheets was proposed to illustrate the photocatalytic process, where the holes accumulated in Bi 2 WO 6 ultrathin nanosheets and O 2 − produced on metallic NPs synergistically promote the selective oxidation of aromatic alcohols.
研究领域:
材料科学
·
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
NANOTECHNOLOGY
·
2023
·Vol. 34
·期 44
·445601
·
IF 3.5
Shuyuan Xu,Bingbao Mei,Fengjiao Li,Jianing Mao,Changxing Huang,Yufeng Yan,Ningning Chen,Yinghua Xu,Meiqin Shi
The application of electrochemical hydrodechlorination has been impeded due to the low utilization and activity of Pd catalyst. Herein, a series of Pd catalysts were prepared via the controllable evolution of Zn state during the pyrolysis of ZIF-8 nanosheet. Various forms of Pd with different chemical surroundings were generated upon the combined use of galvanic displacement and ion exchange process. Electrocatalytic hydrodechlorination of 4-chlorophenol was performed and the electrocatalytic hydrodechlorination efficiency of Pd/CN reaches 100% within 3 h at extra low Pd concentration. The coexistence of zero-valent Pd (Pd0) and nitrogen coordinated Pd (Pd–N) was verified by XAFS which provide multiple active sites for focusing on adsorbing H* and cracking C–Cl respectively. The synergetic effect between different chemical state of Pd for efficient hydrodechlorination of chloroaromatics and scheme for dexterous preparation of Pd based electrocatalyst are proposed and discussed.
研究领域:
环境科学
·
催化化学
✓ 已验证
DOI
高影响因子
JOURNAL OF MEDICINAL CHEMISTRY
·
2025
·
IF 6.8
Hang Zhang,Yujie Zhang,Yinping Geng,Xuanlong Zhen,Xiaodi Wang,Qiange Yin,Peng Zhang,Yuanyuan Li,Mengzhen Zhang,Yi-chao Zheng,Bing-rui Liu,Hui-min Liu,Hai-wei Xu
Gastric cancer is one of the major health threats to human beings and has a low response rate to emerging immunotherapy. We herein reported a novel indole-based LSD1-targeted antigastric agent 7ae, which was able to enhance the sensitivity of gastric cancer cells to a T-cell-mediated immune response. It exhibited potent LSD1 inhibitory activity (IC50 = 0.080 ± 0.002 μM) and reduced the expression of PD-L1, which in turn promoted the T-cell killing response in gastric cancer cells. As a result, 7ae acted as an active LSD1 inhibitor, exerting excellent anti-invasion and anti-migration effects in gastric cancer cells and leading to significant suppression of the growth of xenograft gastric tumors without obvious toxicity in vivo. Collectively, 7ae has been demonstrated to be a novel, potent LSD1 inhibitor with the potential to be used as an antigastric agent, as well as a useful tool compound for exploratory studies of T-cell-mediated immunity and/or immunotherapy in gastric cancer.
研究领域:
肿瘤学
·
药理学
·
免疫学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Cancer Nanotechnology
·
2024
·Vol. 15
·期 1
·1-16
·
IF 4.5
Jiang Qiping,Yao Fengjiao,An Yacong,Lai Xialian,Li Xundou,Yu Zhen,Yang Xian-Da
Background PD-1/PD-L1 blockade plays a crucial role in cancer immunotherapy. Exploration of new technologies to further enhance the efficacy of PD-1/PD-L1 blockade is therefore of potential medical importance. Nanotherapeutics can accumulate in tumor tissues due to enhanced permeability and retention (EPR) effects. In this study, a novel nanotherapeutic for cancer immunotherapy was implemented with albumin nanoparticles functionalized by both PD-1 and PD-L1 aptamers.Results Albumin nanoparticles (NP) were functionalized with either PD-1 aptamers (PD1-NP), PD-L1 aptamers (PDL1-NP), or both types of aptamers (PD1-NP-PDL1). Average sizes of PD1-NP, PDL1-NP, and PD1-NP-PDL1 were 141.8 nm, 141.8 nm, and 164.2 nm, respectively. PD1-NP had good affinity for activated T cells that expresses PD-1. Similarly, PDL1-NP could bind with MDA-MB-231 or CT26 tumor cells that express PD-L1. Moreover, the bispecific PD1-NP-PDL1 could bind with both the activated T cells and the PD-L1-expressing tumor cells, and tether the two type of cells together. Functionally, aptamer-modified nanoparticles exhibited stronger immune-stimulating effects vs. free aptamers. Specifically, PD1-NP or PDL1-NP induced stronger lymphocyte-mediated cytotoxicity against PD-L1-expressing tumor cells in vitro vs. free PD-1 or PD-L1 aptamers. Animal studies also showed that PD1-NP or PDL1-NP significantly improved antitumor efficacy against CT26 colon cancer in vivo vs. free PD-1 or PD-L1 aptamers. Importantly, the bispecific PD1-NP-PDL1 further boosted the in vivo antitumor efficacy compared with PD1-NP or PDL1-NP, without raising systemic toxicity.Conclusion The results suggest that the bispecific PD1-NP-PDL1 is a promising nanotherapeutic to improve the efficacy of PD-1/PD-L1 blockade, and may have application potential in colon cancer treatment.
研究领域:
肿瘤学
·
纳米医学
·
免疫学
✓ 已验证
DOI
高影响因子
JOURNAL OF CATALYSIS
·
2016
·
IF 7.354
Xuelin Zou,Zebao Rui,Shiqi Song,Hongbing Ji
Poor durability and low Pd utilization efficiency are the main drawbacks of supported Pd catalysts for low-temperature methane combustion. Here, we present a facile way to stabilize the performance of Pd/Al 2 O 3 by introducing a spinel NiAl 2 O 4 interface as a promoter at no cost to the activity. The NiAl 2 O 4 interface is formed by impregnation of alumina supports in the nickel-containing solution, followed by high-temperature calcination. A series of 0.4 wt.% Pd/ x NiO/γ-Al 2 O 3 with NiO loading varying among 0.0, 0.5, 1.0, and 9.0 wt.% is investigated. The formation of a NiAl 2 O 4 interface promotes the distribution and crystallization of PdO, suppresses PdO particles aggregation and surface OH − species accumulation during the reaction, and finally leads to the excellent performance of Pd/0.5NiO/γ-Al 2 O 3 . Pd/0.5NiO/γ-Al 2 O 3 demonstrates higher Pd utilization efficiency than the state-of-the-art Pd-based catalysts and better stability than Pd/Al 2 O 3 . Such a spinel interface promotion strategy may bring new insight into the design of highly efficient Pd-based catalysts and their potential technological applications.
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
Journal of the American Chemical Society
·
2023
·
IF 15
Xuan Huang,Bingyan Xu,Jie Feng,Shengnan Hu,Wenjie Dou,Tang Yang,Changhong Zhan,Shangheng Liu,Yujin Ji,Youyong Li,Chih-Wen Pao,Zhiwei Hu,Qi Shao,Xiaoqing Huang
Phase regulation of noble metal-based nanomaterials provides a promising strategy for boosting the catalytic performance. However, realizing the continuous phase modulation in two-dimensional structures and unveiling the relevant structure-performance relationship remain significant challenges. In this work, we present the first example of continuous phase modulation in a library of Pd–Te hexagonal nanoplates (HNPs) from cubic-phase Pd4Te, rhombohedral-phase Pd20Te7, rhombohedral-phase Pd8Te3, and hexagonal-phase PdTe to hexagonal-phase PdTe2. Notably, the continuous phase regulation of the well-defined Pd–Te HNPs enables the successful modulation of the distance between adjacent Pd active sites, triggering an exciting way for tuning the relevant catalytic reactions intrinsically. The proof-of-concept oxygen reduction reaction (ORR) experiment shows a Pd–Pd distance-dependent ORR performance, where the hexagonal-phase PdTe HNPs present the best electrochemical performance in ORR (mass activity and specific activity of 1.02 A mg–1Pd and 1.83 mA cm–2Pd at 0.9 V vs RHE). Theoretical investigation reveals that the increased Pd–Pd distance relates to the weak *OH adsorption over Pd–Te HNPs, thus contributing to the remarkable ORR activity of PdTe HNPs. This work advances the phase-controlled synthesis of noble metal-based nanostructures, which gives huge impetus to the design of high-efficiency nanomaterials for diverse applications.
研究领域:
材料科学
·
电化学
·
纳米技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF CHEMICAL PHYSICS
·
2023
·Vol. 159
·期 12
·
IF 4.4
Liu Huimin,Yuan Chenyi,Wu Shipeng,Sun Chao,Huang Zhen,Xu Hualong,Shen Wei
Surface property modification of catalyst support is a straightforward approach to optimize the performance of supported noble metal catalysts. In particular, oxygen vacancies and hydroxyl groups play significant roles in promoting noble metal dispersion on catalysts as well as catalytic stability. In this study, we developed a nanoflower-like TiO 2 -supported Pd catalyst that has a higher concentration of oxygen vacancies and surface hydroxyl groups compared to that of commercial anatase and P25 support. Notably, due to the distinctive structure of the nanoflower-like TiO 2 , our catalyst exhibited improved dispersion and stabilization of Pd species and the formation of abundant reactive oxygen species, thereby facilitating the activation of CO and O 2 molecules. As a result, the catalyst showed remarkable efficiency in catalyzing the low-temperature CO oxidation reaction with a complete CO conversion at 80 °C and stability for over 100 h.
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-10
·
IF 14.7
Wang Jinlin,Shi Jiangjian,Yin Kang,Meng Fanqi,Wang Shanshan,Lou Licheng,Zhou Jiazheng,Xu Xiao,Wu Huijue,Luo Yanhong,Li Dongmei,Chen Shiyou,Meng Qingbo
Charge loss at grain boundaries of kesterite Cu 2 ZnSn(S, Se) 4 polycrystalline absorbers is an important cause limiting the performance of this emerging thin-film solar cell. Herein, we report a Pd element assisted reaction strategy to suppress atomic vacancy defects in GB regions. The Pd, on one hand in the form of PdSe x compounds, can heterogeneously cover the GBs of the absorber film, suppressing Sn and Se volatilization loss and the formation of their vacancy defects (i.e. V Sn and V Se ), and on the other hand, in the form of Pd(II)/Pd(IV) redox shuttle, can assist the capture and exchange of Se atoms, thus contributing to eliminating the already-existing V Se defects within GBs. These collective effects have effectively reduced charge recombination loss and enhanced p-type characteristics of the kesterite absorber. As a result, high-performance kesterite solar cells with a total-area efficiency of 14.5% (certified at 14.3%) have been achieved.
研究领域:
材料科学
·
太阳能
·
半导体物理
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF CATALYSIS
·
2022
·
IF 8.047
Xiaodong Zhang,Fukun Bi,Zhenyuan Zhao,Yang Yang,Yintao Li,Liang Song,Ning Liu,Jingcheng Xu,Lifeng Cui
Supported single-atoms and sub-nanometre clusters have exhibited superb catalytic performance toward many reactions. However, inactivation of single-atom or cluster catalysts in complex reactive conditions poses major challenge for their practical application. Herein, we demonstrate that the prepared Pd-UiO-66 with ultra-low Pd loading (0.05 wt%) contains three robust active Pd species, (isolated Pd atom (Pd 1 ), sub-nanometre Pd clusters (Pd c ) and Pd nanoparticles (Pd n )) and presents superb activity for toluene oxidation and water resistance (10.0 vol%). Experiments and theoretical calculations firstly confirm that consecutive H 2 -O 2 and reaction gas treatment (1000 ppm toluene in 20 vol.%O 2 /Ar) induce residual N species from solvent N, N-dimethylformamide to enter UiO-66 skeleton forming Pd 1 -N 1 structures. DFT calculations reveal that the synergistic effect of Pd species (namely, the enhanced activation of O 2 and H 2 O by Pd 1 and the improved adsorption of toluene by Pd c and Pd n ) is the main factor for the excellent activity of Pd-U-H-O-reused catalyst.
研究领域:
催化化学
·
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
CANCER CELL
·
2022
·
IF 38.585
Haixia Long,Qingzhu Jia,Liuyang Wang,Wenfeng Fang,Zhongyu Wang,Tao Jiang,Fei Zhou,Zheng Jin,Jiani Huang,Li Zhou,Chunyan Hu,Xinxin Wang,Jin Zhang,Yujie Ba,Yujie Gong,Xianghua Zeng,Dong Zeng,Xingxing Su,Peter B. Alexander,Li Wang,Limei Wang,Yisong Y. Wan,Xiao-Fan Wang,Li Zhang,Qi-Jing Li,Bo Zhu
Summary Despite the unprecedented success of immune checkpoint inhibitors (ICIs) as anti-cancer therapy, it remains a prevailing clinical need to identify additional mechanisms underlying ICI therapeutic efficacy and potential drug resistance. Here, using lineage tracking in cancer patients and tumor-bearing mice, we demonstrate that erythroid progenitor cells lose their developmental potential and switch to the myeloid lineage. Single-cell transcriptome analyses reveal that, notwithstanding quantitative differences in erythroid gene expression, erythroid differentiated myeloid cells (EDMCs) are transcriptionally indistinguishable from their myeloid-originated counterparts. EDMCs possess multifaceted machinery to curtail T cell-mediated anti-tumor responses. Consequently, EDMC content within tumor tissues is negatively associated with T cell inflammation for the majority of solid cancers; moreover, EDMC enrichment, in accordance with anemia manifestation, is predictive of poor prognosis in various cohorts of patients undergoing ICI therapy. Together, our findings reveal a feedforward mechanism by which tumors exploit anemia-triggered erythropoiesis for myeloid transdifferentiation and immunosuppression.
研究领域:
肿瘤学
·
免疫学
·
分子生物学
·
癌症治疗
✓ 已验证
DOI
PubMed
高影响因子
ACS Applied Nano Materials
·
2023
·
IF 5.9
Lulu Kong,DeZhu Chen,Xiaolong Zhang,Lin Zhou,Yongming Deng,Shaohua Wei
The growth of oxides on the surface of noble metals and the introduction of alloys are effective methods to enhance the catalytic activity of noble metals. However, the fabrication of noble metal oxides always involves harsh experimental conditions and the oxidation degree could not be controlled. Herein, a simple, fast, and controlled Pd oxidation method by mixing Hg2+ and Pd nanosheets (PdNSs) under mild conditions to form PdxHgy(PdO)z (PHOs) was reported, which consists of the Pd–Hg alloy and PdO. The density functional theory (DFT) calculation and experiment results proved that the Hg atom incorporation promotes the nearby Pd–Pd bond breaking, initiating a cascade of PdO generation. More precisely, 1 Hg atom incorporation induced ∼8 Pd atom oxidation, ensuring that the oxidation degree of Pd could be easily controlled by adjusting the ratio of Hg2+ and PdNS. As a peroxidase-mimicking nanozyme, the PHO affinity for its substrate could be 21.7- and 123.6-fold greater than that of the PdNS and the natural peroxidase (HRP), respectively. For the colorimetric immunoassay of carcinoembryonic antigen (CEA) detection, PHO has an ultralow detection limit of 1.33 pg mL–1, which is ∼8.6 and ∼282 times lower than that of the PdNS and the natural HRP, respectively.
研究领域:
生物化学
·
医学诊断
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2023
·
IF 8.2
Qiuyang Huang,Xiaoling Zang,Zhiwei Zhang,Hang Yu,Baoyan Ding,Zhuangzhuang Li,Simin Cheng,Xin Zhang,Mustafa R.K. Ali,Xue Qiu,Zhihua Lv
The discovery of new anti-cancer drugs targeting the PD-1/PD-L1 pathway has been a research hotspot in recent years. In this study, biological affinity ultrafiltration (BAU), UPLC-HRMS, molecular dynamic (MD) simulations and molecular docking methods were applied to search for endogenous active compounds that can inhibit the binding of PD-L1 to PD-1. We screened dozens of potential cancer related endogenous compounds. Surprisingly, cyclic adenosine monophosphate (cAMP) was found to have a direct inhibitory effect on the PD-1/PD-L1 binding with an in vitro IC 50 value of about 36.4 ± 9.3 μM determined by homogeneous time-resolved fluorescence (HTRF) assay. cAMP could recover the proliferation of Jurkat T cells co-cultured with DU-145 cells and may suppress PD-L1 expression of DU-145 cells. cAMP was demonstrated to bind and induce PD-L1 dimerization by FRET assay, and also predicted by MD simulations and molecular docking. The finding of cAMP as a potential inhibitor directly targeting the PD-1/PD-L1 interaction could advance our understanding of the activity of endogenous compounds regulating PD-L1.
研究领域:
肿瘤学
·
药理学
·
分子生物学
·
细胞生物学
✓ 已验证
产品关联
DOI
PubMed
高影响因子