CATALYSIS LETTERS
·
2021
·Vol. 151
·期 10
·3004-3010
·
IF 3.186
Zhou Junjie,Huang Yu,Shen Jialu,Liu Xiang
The production of H 2 from non-fossil sources is a key research challenge to contributing solving the forthcoming energy problem. Aqueous solutions of tetrahydroxydiboron have very recently appeared as a H 2 source, from which both hydrogen atoms are provided by water, in the presence of highly sophisticated nanocatalysts. Herein, commercial and cheap Pd/C is shown to be an efficient and recyclable catalyst for H 2 evolution upon tetrahydroxydiboron hydrolysis. Graphic Abstract
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2020
·
IF 16.683
Jia-Fang Xie,Jie-Jie Chen,Yu-Xi Huang,Xing Zhang,Wei-Kang Wang,Gui-Xiang Huang,Han-Qing Yu
In this work, a novel Cu-Pd heterostructure, derived from CuCl-PdO x hexagonal microplates, was prepared to tune selective single hydrocarbon production from electrochemical CO 2 reduction. The CuCl-PdO x hexagonal microplates were synthesized by a dual-potential electrodeposition technique, followed by electrochemical reduction to form Cu-Pd heterostructure. This Cu-Pd heterostructure exhibited a much higher CO 2 -to-CH 4 selectivity (32 % Faradaic efficiency, FE) compared to pure Cu or Pd. Moreover, Cu-Pd heterostructure showed excellent suppression on C 2 H 4 generation (below 1 % FE). The density functional theory calculations suggested that the hollow site of Pd region in the Cu-Pd heterostructure could stablize CO* intermediate and selectively lowered the energy demand for CH 4 formation rather than C 2 H 4 . This work provides new opportunities of designing Cu-based electrocatalysts for selective CO 2 reduction to single hydrocarbon.
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Chemosensors
·
2024
·Vol. 12
·期 3
·43
·
IF 3.7
Yi Li,Boyu Zhang,Juan Li,Zaihua Duan,Yajie Yang,Zhen Yuan,Yadong Jiang,Huiling Tai
The NH3sensor is of great significance in preventing NH3leakage and ensuring life safety. In this work, the Pd-decorated ZnO hexagonal microdiscs are synthesized using hydrothermal and annealing processes, and the gas sensor is fabricated based on Pd-decorated ZnO hexagonal microdiscs. The gas-sensing test results show that the Pd-ZnO gas sensor has a good response to NH3gas. Specifically, it has a good linear response within 0.5–50 ppm NH3at the optimal operating temperature of 230 °C. In addition, the Pd-ZnO gas sensor exhibits good repeatability, short response time (23.2 s) and good humidity resistance (10–90% relative humidity). This work provides a useful reference for developing an NH3sensor.
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Nanomaterials
·
2021
·Vol. 11
·期 11
·3028
·
IF 5.076
Tingting Cao,Jinke Cheng,Jun Ma,Chunliang Yang,Mengqin Yao,Fei Liu,Min Deng,Xiaodan Wang,Yuan Ren
Formic acid (FA) is found to be a potential candidate for the storage of hydrogen. For dehydrogenation of FA, the supports of our catalysts were acquired by conducting ZnCl2treatment and carbonation for biomass waste. The texture and surface properties significantly affected the size and dispersion of Pd and its interaction with the support so as to cause the superior catalytic performance of catalysts. Microporous carbon obtained by carbonization of ZnCl2activated peanut shells (CPS-ZnCl2) possessing surface areas of 629 m2·g−1and a micropore rate of 73.5%. For ZnCl2activated melon seed (CMS-ZnCl2), the surface area and micropore rate increased to 1081 m2·g−1and 80.0%, respectively. In addition, the introduction of ZnCl2also caused the increase in surface O content and reduced the acidity of the catalyst. The results represented that CMS-ZnCl2with uniform honeycomb morphology displayed the best properties, and the as-prepared Pd/CMS-ZnCl2catalyst afforded 100% hydrogen selectivity as well as excellent catalytic activity with an initial high turnover number (TON) value of 28.3 at 30 °C and 100.1 at 60 °C.Keywords:porous carbon;Pd nano-catalysts;agriculture waste;formic acid;dehydrogenation
研究领域:
材料科学
·
催化化学
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RARE METALS
·
2024
·
IF 9.6
Hu Xiao-Jie,Sun Yu-Han,Liu Ling-Yue,Mao Dan-Jun,Zheng Shou-Rong
Monochloroacetic acid (MCAA) is identified as a highly carcinogenic disinfection by-product in chlorinated drinking water. In this study, a series of CeO 2 -supported Pd catalysts (Pd/MCeO 2 ) were synthesized through one-step calcination of Pd-loaded Ce-UiO-66-BDC (Ce-MOF), and the liquid-phase catalytic hydrodechlorination of MCAA was explored using these catalysts. For comparison, Pd/CeO 2 catalysts were additionally synthesized using the conventional impregnation method. The characterization results reveal that the catalysts exhibit strong metal–support interaction, leading to high Pd dispersion and Pd n + content. Additionally, the calcination temperature significantly influences catalytic performance, with the catalyst calcined at 500 °C (Pd/MCeO 2 -500) demonstrating the highest catalytic activity and achieving complete dechlorination of MCAA within 50 min. Furthermore, it is found that the catalytic MCAA hydrodechlorination using the catalysts adheres to the Langmuir–Hinshelwood model. Accordingly, low reaction pH is favorable for the catalytic hydrodechlorination of MCAA, enhancing MCAA adsorption on the catalyst surface due to the electrostatic interaction between MCAA and the catalyst surface. Theoretical results suggest that the presence of Pd n + efficiently facilitates MCAA adsorption and C–Cl cleavage, thus significantly enhancing the liquid-phase catalytic hydrodechlorination. Graphical abstract
研究领域:
环境科学
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催化化学
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材料科学
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Chem
·
2025
·Vol. 12
·期 3
·
IF 19.6
Yu-He Liang,Jia-Xin Kang,Yan Wang,Yi-Ge Li,Hou-Ji Cao,Qianyi Zhao,Xuenian Chen,Yan-Na Ma
The selective B–H functionalization of carboranes has received considerable attention because of their wide applications in functional materials, catalysis, and pharmaceuticals. Deuterium-labeling experiments and kinetic-isotope-effect experiments are two important tools for mechanistic studies on the selective B–H activation of carboranes. Thus, developing an effective method for the synthesis of perdeuterated carboranes is highly desirable. Herein, we present a practical method for synthesizing perdeuterated carboranes via Pd(II)-catalyzed B–H activation by using D 2 O as a deuterium source. This protocol features extraordinary functional-group tolerance, high levels of deuterium incorporation, and ease of scaling. Mechanistic studies illustrate that the deuteration reaction proceeds via Pd(II)-catalytic electrophilic H/D exchange and subsequent intermolecular Pd migration. The same degree of deuterium incorporation across all boron vertices indicates that the Pd-migration step is faster than the electrophilic palladation step. Additionally, the versatility of this method is reflected in the deuteration of other boron clusters.
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Experimental Hematology & Oncology
·
2025
·Vol. 14
·期 1
·1-17
·
IF 13.5
Ren Xueting,Wu Jinpeng,Li Jing,Zhai Zhen,Li Xiang,Guan Feng,Wang Meng,Ma Xiaobin,Tan Zengqi,Kang Huafeng,Lin Shuai
Background The abundance of PD-L1 on the surface of tumor cells is a critical factor in sensitizing these cells to T cell-mediated immune killing. While abnormal glycosylation of PD-L1 is known to influence its expression and function, the precise regulatory mechanisms remain unclear.Methods This study utilized bioinformatics analysis to explore the role of MGAT3, a key gene involved in the formation of the bisecting GlcNAc structure, in breast cancer (BC). Experimental approaches were employed to increase bisecting GlcNAc levels in BC cells, followed by assessments of PD-L1 expression, CD8+ T cell-mediated cytotoxicity, extracellular vesicle (EV)-associated PD-L1, and PD-L1/PD-1 interaction. Additionally, forskolin, a bisecting GlcNAc agonist, was combined with anti-PD-L1 antibody to evaluate its antitumor effects in vivo.Results MGAT3 was found to be expressed at low levels in BC tissues but positively correlated with CD8+ T cell infiltration. Elevating bisecting GlcNAc levels in BC cells significantly enhanced the cytotoxic efficacy of CD8+ T cells. High bisecting GlcNAc modification promoted PD-L1 degradation via the lysosomal pathway, reducing PD-L1 expression and its binding to PD-1. Furthermore, increased bisecting GlcNAc levels reduced PD-L1 in tumor cell-derived EVs, impairing the EVs’ ability to block CD8+ T cells and indirectly enhancing T cell cytotoxicity. The combined use of forskolin and anti-PD-L1 antibody significantly increased CD8+ T cell abundance and activity, achieving a more effective antitumor response in vivo.Conclusion sThese findings demonstrate that enhancing bisecting GlcNAc modification in BC cells promotes PD-L1 degradation and inhibits its binding to PD-1, thereby boosting CD8+ T cell-mediated cytotoxicity, providing a promising strategy for immune modulation in BC therapy.
研究领域:
癌症生物学
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免疫学
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生物化学
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糖生物学
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分子生物学
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PubMed
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NANO
·
2026
·
IF 1.1
Shimeng Chang,Yuting Sun,Jiuyang Lin,Yao Weng,Shuping Zhang,Fengyang Jing,Wenjing Yuan
Formaldehyde (HCHO), as a typical organic pollutant, seriously threatens human health. Room-temperature catalytic oxidation can effectively convert HCHO into CO 2 and H 2 O, however, it still faces the problem of low catalytic efficiency. In this study, the CeO 1-y Cl/Pd catalysts were constructed to propose a synergistic HCHO capture-mineralization strategy based on the interaction between oxygen vacancies and Pd active sites. The surface oxygen vacancies of CeO 1-y Cl enable efficient HCHO adsorption through strong interactions with the carbonyl oxygen of HCHO, and meanwhile the Pd active sites activate O 2 to generate superoxide radicals (°O 2- ) driving the deep oxidation of adsorbed HCHO. The substitution of lattice oxygen of CeO 2 by chloride ions not only stabilizes oxygen vacancies but also significantly enhances the dispersion of Pd active sites. The experimental results indicate that the typical sample (CeO 1-y Cl/Pd-6) exhibit the excellent catalytic oxidation efficiency for HCHO, with remove rate of 79.1 %. This study provides a feasible solution to design efficient catalysts for purification of HCHO pollution.
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Chemistry-An Asian Journal
·
2021
·Vol. 16
·期 19
·2952-2957
·
IF 4.568
Fengwei Zhang,Mengmeng Liu,Qiang Liu,Jingjing Li,Boyang Li,Zhengping Dong
Graphical A facile and in-situ methanol-mediated strategy was proposed to fabricate Pd@ZIF-8 catalyst for efficient and size-selectivity alkenes hydrogenation. In-situ encapsulation of tiny and well-dispersed Pd nanoparticles (Pd NPs) in zeolitic imidazolate frameworks (ZIFs) was firstly achieved using a one-pot and facile methanol-mediated growth approach, in which methanol served as both solvent and a mild reductant. The microstructure, morphology, crystallinity, porosity as well as evolution process of the catalysts were determined by TEM, XRD, N 2 adsorption and UV-vis spectra. Due to the complete encapsulation of such Pd NPs combined with ultrahigh surface area and uniform microporous structure of ZIF-8, the resulting Pd@ZIF-8-60 min nanocomposite exhibited more superior catalytic activity for olefins hydrogenation with TOF of 7436 h −1 and excellent size selectivity than previously reported catalysts. Furthermore, the catalyst displays excellent recyclability for 1-octene hydrogenation and without any loss of the Pd active species.
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APPLIED CATALYSIS A-GENERAL
·
2015
·
IF 3.942
Qunfeng Zhang,Wei Xu,Xiaonian Li,Dahao Jiang,Yizhi Xiang,Jianguo Wang,Jie Cen,Stephen Romano,Jun Ni
The preparation of supported palladium sulfides catalysts has attracted much attention due to their good sulfur-resistant properties in the hydrogenation of sulfur-containing compounds. In this work, we unambiguously demonstrated that Pd/C catalyst could be in situ sulfided by organic sulfur-containing reactant molecules and the sulfidation was highly dependent on temperature. The in situ sulfidation of Pd/C catalyst was composed of a reaction of Pd with the sulfur derived from the cleavage of C S bond of sulfur-containing reactant molecules, followed by a transformation to Pd x S y at high temperatures (around 120 °C). The sulfided Pd/C catalyst could be used for at least 18 recycles without a significant loss in its activity during the hydrogenation of sulfur-containing nitrobenzene at 180 °C with 3 MPa H 2 , which could be attributed to the stable presence of Pd 4 S and Pd 16 S 7 .
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ChemistrySelect
·
2024
·Vol. 9
·期 1
·e202303384
·
IF 1.9
Shiqin Lai,Zhibing Kang,Lie-Yuan Zhang,Dengke Wang,Lanqing Deng,Jian-Ping Zou
Graphical Ultrafine Pd nanoparticles (1.41 nm)-embedded MIL-100(Fe) (Pd-MOF-Fe) nanocomposites are synthesized via a double-solvent impregnation integrated with photo-reduction approach. Coupling MOF-based catalysis with Pd-based catalysis, the resultant Pd-MOF-Fe shows excellent catalytic efficiency and high stability toward visible-light-induced dehydrogenation of alcohols to hydrogen evolution and value-added carbonyl chemical production. Solar-driven hydrogen (H 2 ) evolution combined with synchronously selective oxidation for fine chemicals production is of great significance in energy and synthetic chemistry. Herein, ultrafine Pd nanoparticles-encapsulated MIL-100(Fe) (Pd-MOF-Fe) nanocomposites are synthesized through double-solvent impregnation integrated with photo-reduction method. Integrating MOF-based catalysis and Pd-based catalysis, the Pd-MOF-Fe can serve as multifunctional catalyst for photoinduced alcohol dehydrogenation reaction. Optimal generation rates of H 2 (3.61 mmol g −1 h −1 ) and benzaldehyde (3.40 mmol g −1 h −1 ) are gained over Pd-MOF-Fe, ca. 4.1 times that of the Pd/MOF-Fe, in which Pd crystals with size ranging from 3 to 6 nm are immobilized on the intersurface of MOFs. Besides, controlled experiments reveal the pivotal role of the opened FeO 6 nodes of MIL-100(Fe) as Lewis acid sites toward alcohol activation. This work provides a controllable approach for metal nanoparticle immobilization. Furthermore, considering the diversified MOF structures, this study also highlights the infinite possibility of metal nanoparticle/MOFs as multifunctional platform for solar energy conversion and chemicals production.
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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.
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