ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Shuchao Jiang,Hongqi Shi,Yuzhe Xu,Jiaojiao Liu,Tie Yu,Guoqing Ren
Formic acid (FA, HCOOH) is regarded as one of the most promising carriers for hydrogen storage. However, the catalyst design for FA dehydrogenation into H2 with high efficiency is not clear. Here, we elucidate the rationale of size effect over the most commonly used Pd-based catalyst through supporting different Pd species, including single atoms, nanoclusters, and nanoparticles, on amine-functionalized active carbon (Pd/AC-NH2). The activity test presents that Pd/AC-NH2 with Pd nanoclusters exhibits the best turnover frequency (TOF) value of 40856 h–1 for 1 M FA at 328 K and even 1504 h–1 for neat FA at 308 K, which is comparable to the homogeneous catalysts and has been the first heterogeneous catalyst used in neat FA dehydrogenation under mild conditions. The comprehensive characterizations reveal that the size of Pd species affects the ratios of Pd0/Pd2+ and hydrogen spillover effect, which is crucial for the C–H cleavage and H2 desorption. Besides, the influences of amine groups on catalytic performance were further examined. This work provided an ingenious guideline to design efficient and practical catalysts for hydrogen storage under ambient conditions.
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APPLIED SURFACE SCIENCE
·
2025
·
IF 6.9
Yanan Wei,Tao Xia,Tongyu Zhong,Henghui Zhu,Yucai He,Yunlei Zhang
Interface engineering is a significance strategy to afford efficient selective oxidation for supported catalysts. Herein, constructing of frustrated Lewis pairs (FLPs) sites on CeO 2 and supporting Au-Pd nanoparticles to provide a highly selective production of 2,5-furandicarboxylic acid (FDCA) from 2,5-bis(hydroxymethyl)furan (BHMF). Mechanism investigations illustrate that the FLPs active sites enhance the adsorption and activation of catalyst for BHMF, decreasing the activation energy of rate-determining step. Simultaneously, the FLPs sites induce the electron transfer of the catalyst, generating a novel Au-Pd-CeO 2 interface that promotes the adsorption of molecule oxygen and the formation of the superoxide radical. Thereby, the Au x Pd y /P T -CeO 2 catalysts enable superior catalytic performance, achieving a satisfactory turnover frequency of 55.29 h −1 and a highly FDCA yield of 94.0 %. Such interfacial FLPs sites exhibit the great potentials for the selective oxidation of various unsaturated compounds.
研究领域:
化学工程
·
催化科学
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STAR Protocols
·
2021
·
IF 0
Zhengxin Peng,Man Yu,Jiaming Lin,Tianqi Dong,Xiao Zhang,Mingjun Shi,Min Qin,Shasha Li,Wencong Guo,Huixia Zhang,Shuguo Sun
Summary Anti-PD-1/PD-L1 therapy shows long-term effects in many cancer types, but resistance and relapse remain the main limitations of this therapy. Here, we describe a protocol to evaluate the tumor response to immunotherapy in a mouse lung cancer model. The protocol includes the establishment of the lung cancer mouse model, anti-PD-1 treatment, tumor-infiltrating lymphocyte isolation, immunofluorescence, and flow cytometry analysis. This protocol can also be applied to other cancer types and immunotherapies. For complete details on the use and execution of this protocol, please refer to Yu et al. (2021)
研究领域:
肿瘤学
·
免疫学
·
分子生物学
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Science Advances
·
2024
·Vol. 10
·期 40
·
IF 11.7
Feng Zhang,Qiuyu Jiang,Jialiang Cai,Fansheng Meng,Wenqing Tang,Zhiyong Liu,Xiahui Lin,Wenfeng Liu,Yi Zhou,Xizhong Shen,Ruyi Xue,Ling Dong,Si Zhang
The efficacy of immunotherapy targeting the PD-1/PD-L1 pathway in hepatocellular carcinoma (HCC) is limited. NOD-like receptors (NLRs) comprise a highly evolutionarily conserved family of cytosolic bacterial sensors, yet their impact on antitumor immunity against HCC remains unclear. In this study, we uncovered that NOD1, a well-studied member of NLR family, exhibits predominant expression in tumor-associated macrophages (TAMs) and correlates positively with improved prognosis and responses to anti–PD-1 treatments in patients with HCC. Activation of NOD1 in vivo augments antitumor immunity and enhances the effectiveness of anti–PD-1 therapy. Mechanistically, NOD1 activation resulted in diminished expression of perilipin 5, thereby hindering fatty acid oxidation and inducing free fatty acid accumulation in TAMs. This metabolic alteration promoted membrane localization of the costimulatory molecule OX40L in a lipid modification–dependent manner, thereby activating CD8+ T cells. These findings unveil a previously unrecognized role for NOD1 in fortifying antitumor T cell immunity in HCC, potentially advancing cancer immunotherapy.
研究领域:
肿瘤学
·
免疫学
·
癌症生物学
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2026
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IF 6.7
Min Sun,Yihu Zhang,Siyu Chu,Yifan Ma,Bin Li,Haiyan Wang,Shiquan Feng,Yong Wang,Yongguang Huang,Yachuan Liang,Zijiong Li
The large-scale deployment of alkaline fuel cells is still hindered by the sluggish cathodic oxygen reduction reaction (ORR) and the high cost of Pt-based catalysts. Herein, interconnected Pd/carbon-dot (Pd/CD) nanowires were fabricated through an oxalic-acid-assisted coordination strategy coupled with temperature-controlled reduction for efficient alkaline ORR. Nitrogen-doped carbon dots provide abundant anchoring sites for Pd species, while oxalic acid provides a mild reducing environment and coordinates with Pd 2+ through carboxylate groups. This process regulates Pd nucleation and growth, suppresses aggregation, and promotes interfacial electronic coupling. The catalyst prepared at 40 °C exhibits a well-dispersed, interconnected nanowire architecture with abundant accessible active sites. It delivers an onset potential of 0.996 V and a half-wave potential of 0.878 V, outperforming commercial Pt/C under identical testing conditions. X-ray absorption fine structure analysis and density functional theory calculations suggest that strong Pd–CD interfacial coupling optimizes the adsorption energetics of key oxygenated intermediates and reduces the ORR energy barrier. This work provides a coordination-regulated strategy for designing efficient Pd-based electrocatalysts for alkaline fuel-cell applications.
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Nano Research
·
2021
·Vol. 15
·期 4
·2928-2934
·
IF 8.897
Xiao Xudong,Lin Siying,Zhang Liping,Meng Huiyuan,Zhou Jing,Li Qi,Liu Jianan,Qiao Panzhe,Jiang Baojiang,Fu Honggang
The formation of chemical bonds between metal ions and their supports is an effective strategy to achieve good catalytic activity. However, both the synthesis of active metal species on a support and control of their coordination environment are still challenging. Here, we show the use of an organic compound to produce tubular carbon nitride (TCN) as a support for Pd nanoparticles (NPs), creating a composite material (NP-Pd-TCN). It was found that Pd ions preferentially bind with the electron-rich N atoms of TCN, leading to strong metal-support interactions that benefit charge transfer from g-C 3 N 4 to Pd. X-ray absorption spectroscopy further revealed that the metal-support interactions resulted in the formation of Pd-N bonds, which are responsible for the improvement in the charge dynamics as evidenced by the results from various techniques including photoluminescence (PL) spectroscopy, photocurrent measurements, and electrochemical impedance spectroscopy (EIS). Owing to the good dynamical properties, NP-Pd-TCN was used for photocatalytic hydrogen evolution under visible-light irradiation ( λ > 420 nm) and an excellent evolution rate of ∼ 381 µmol·h −1 (0.02 g of the photocatalyst) was attained. This work aims to promote a strategy to synthesize efficient photocatalysts for hydrogen production by controllably introducing metal nanoparticles on a support and in the meantime forming chemical bonds to achieve intimate metal-support contact.
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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.
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Journal of Materials Chemistry A
·
2015
·Vol. 3
·期 21
·11261-11268
·
IF 7.443
Jing Li,Panpan Zhou,Feng Li,Ren Ren,Yang Liu,Jianrui Niu,Jianxin Ma,Xueyao Zhang,Min Tian,Jun Jin,Jiantai Ma
In the present work, nickel (Ni) and palladium (Pd) core–shell structure nanospheres with various thicknesses have been facilely obtained via a one-pot synthesis process. These hybrid structures allow us to correlate the Pd thickness with their performance in the hydrogen evolution reaction (HER). The HER activity increases with a decrease of the Pd thickness, and it can be ascribed to the enhancement of electron donation of Pd (111) caused by the electron flow from Ni (111) to Pd (111) based on first-principles calculations. In this hybrid system, the difference in work functions of Pd and Ni results in surface polarization on the Pd surface, tuning its charge state for hydrogen reduction. Meanwhile, with the assistance of a polyethyleneimine–reduced graphene oxide (PEI–rGO) support, the examined Ni@Pd4:1/PEI–rGO50:1 (10 wt%) electrocatalyst presents outstanding HER activity comparable with that of platinum (Pt). This work opens up possibilities for reducing Pd usage while achieving high HER performance.
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ChemCatChem
·
2018
·Vol. 10
·期 7
·1620-1626
·
IF 4.674
Wei Wang,Zhang-Hui Lu,Yan Luo,Aihua Zou,Qilu Yao,Xiangshu Chen
Graphical Dispersed Nanoparticles : Highly dispersed PdNi nanoparticles (NPs) have been successfully immobilized on mesoporous carbon nitride (MCN) through a facile co-reduction approach, which shows excellent catalytic performance for hydrogen release from an ammonia borane (AB) aqueous solution at room temperature. Highly dispersed Pd and PdNi nanoparticles (NPs) have been successfully immobilized on mesoporous carbon nitride (MCN) through a facile co-reduction approach. The resulting Pd/MCN catalyst shows excellent catalytic performance for hydrogen release from an ammonia borane (AB) aqueous solution with a turnover frequency (TOF) value of 125 mol H 2 mol metal −1 min −1 at room temperature, which is among the highest values for monometallic Pd-based catalysts reported to date. The catalytic performance of the Pd NPs can be further enhanced by alloying with Ni or Co atoms. Among all the synthesized Pd x Ni 100− x /MCN nanocomposites (NCs) with different Ni/Pd ratios, the Pd 74 Ni 26 /MCN catalyst exhibits the best catalytic performance with a TOF of 246.8 mol H 2 mol metal −1 min −1 . The high activity of Pd/MCN and Pd 74 Ni 26 /MCN are largely dependent on the features of the ultrafine metallic NPs immobilized by MCN, the interfacial interaction between the MCN matrix and metallic NPs, and the accessible open porous structure for mass transfer.
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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.
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ONCOLOGY REPORTS
·
2025
·Vol. 54
·期 1
·1-16
·
IF 3.9
Yubo Yan,Xianglong Kong,Xiangyuan Jin,Jianlong Bu,Boxiong Ni,Zuqin Rao,Junnan Guo,Shidong Xu
Ring finger protein 125 (RNF125), a ubiquitin E3 ligase, has been reported to act as a tumor suppressor in several cancers, but its precise function in lung adenocarcinoma (LUAD) has not been elucidated. In the present study, through bioinformatics analysis and immunohistochemistry in LUAD and non‑cancerous samples, it was demonstrated that RNF125 was significantly downregulated in lung cancer. Low levels of RNF125 expression were associated with metastatic status, advanced tumor stage and poor overall survival in LUAD. The results of gain‑ and loss‑of‑function experiments demonstrated that RNF125 inhibited proliferation, colony formation, migration and invasion of LUAD cells. In addition, RNF125 increased the sensitivity of LUAD cells to cisplatin. Mechanistically, RNF125 interacted with programmed cell death ligand 1 (PD‑L1) and reduced PD‑L1 expression levels in LUAD cells. Furthermore, IL‑2 secretion by Jurkat T cells was significantly suppressed when co‑cultured with RNF125‑silenced LUAD cells. NK‑92 cell lysis of RNF125‑silenced LUAD cells was also weaker compared with that of control LUAD cells, suggesting that RNF125 knockdown enhanced the immune evasion ability of LUAD cells. Notably, the results of the present study identified that the RNA‑binding protein muscleblind‑like 1 (MBNL1) is the upstream regulator of RNF125 in LUAD. MBNL1 increased the stability of the RNF125 transcript in LUAD cells and knockdown of RNF125 reversed the antitumor effect of MBNL1 on LUAD cells. In conclusion, the present study demonstrated the tumor suppressor role of RNF125 in LUAD and implicated MBNL1 as an upstream regulator of RNF125 in LUAD. These findings contributed to an improved understanding of the molecular features of LUAD progression.
研究领域:
肿瘤学
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分子生物学
·
免疫学
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CHEMISTRY-A EUROPEAN JOURNAL
·
2022
·Vol. 29
·期 16
·e202203142
·
IF 5.02
Jingwen Luo,Anqi Huang,Yao-Yue Yang,Xing-Yu Ma,Quan-Liang Chen,Junxian Chen,Yajuan Wu
Graphical Put to good use : A Pd-doped Co (Pd/Co) catalyst with high Pd atom utilization efficiency was designed and prepared for hydrogenation of nitroarenes. Its catalytic activity was much better than commercial Pd powder (>150 times) in nitrobenzene hydrogenation reaction. This work might provide a simple and low-cost methodology to design and synthesize highly efficient catalysts. Enhancing catalytic performance as well as reducing catalyst cost are the eternal pursuit for the catalysis community. Herein, a simple and effective palladium-doped cobalt (Pd / Co) catalyst with high Pd atom utilization efficiency was synthesized via galvanic replacement reaction for the selective hydrogenation of nitrobenzene with H 2 at room temperature, delivering >99 % yield of aniline with up to 158 times higher catalytic activity than commercial palladium powder. Detailed characterizations and DFT calculations revealed that Co−Pd interaction leads to a decrease in electron density of Pd and the distance between Pd atoms that results in the enhanced catalytic performance. Further experiments indicated that the Pd / Co catalyst serves as a highly efficient, selective, and recyclable catalyst for a range of nitroarene substrates. This work might provide a green and sustainable methodology to design and synthesize highly active catalysts with high utilization efficiency of the noble metals in fundamental and applied research.
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