BIOMATERIALS
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2026
·
IF 13.6
Yingtao Zhong,Keyan Zhang,Xinyu Li,Zhuofeng Li,Xinjia Huang,Ziwen Qiu,Junmei Nie,Jiaqi Wang,Shiying Li,Hong Cheng
Despite its critical role in treating localized breast cancer, radiotherapy (RT) rarely provokes systemic immune responses or abscopal effects. In this work, immunological profiling reveals that RT upregulates CD47 and PD-L1 expressions in tumor cells and promotes the accumulation of M2-type tumor-associated macrophages (TAMs), suggesting a potential immunosuppressive mechanism that restricts abscopal responses. To overcome this limitation, a legumain-activated radio-immunological synergist (LARIS) is rationally designed to amplify RT-induced abscopal effects through dual CD47/PD-L1 blockade and TAM repolarization. LARIS is constructed from a bispecific immune checkpoint blockade chimeric peptide (BiCCP) linking CD47-and PD-L1-blocking peptides via a legumain-cleavable linker, and co-formulated with the Toll-like receptor 7/8 agonist R848. Within the tumor microenvironment, abundant legumain can cleave LARIS to release R848 together with the checkpoint blockade peptides, thereby reprogramming TAMs toward an M1 phenotype and mitigating CD47/PD-L1-mediated immune evasion. Both in vitro and in vivo studies demonstrated that LARIS significantly enhances systemic antitumor immunity and effectively induces abscopal responses of RT, thus suppressing the growth of distant and rechallenged tumors. Overall, this work offers a promising strategy to counteract RT-induced immunosuppression and potentiate abscopal effects for improved breast cancer therapy.
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高影响因子
MICROCHEMICAL JOURNAL
·
2026
·
IF 5.2
Honghui Li,Rui Yuan,Lingshuang Peng,Lu Zhang,Jianle Wang,Yuling Li,Yaqi Qin,Dexing Chen,Wenchun Xu,Meiying Shen,Changjin Liu
Pd single-atom loaded PdCoB alloy mesoporous nanospheres (Pd-PdCoB SAMNs) exhibited exceptional peroxidase-like activity. • A electrochemical biosensor was developed using Pd-PdCoB SAMNs and DDA-Cu MOFs nanobelts for H 2 O 2 detection. • The constructed electrochemical biosensor demonstrated outstanding performance in the ultrasensitive detection of H 2 O 2 in cancer cells. Hydrogen peroxide (H 2 O 2 ), a key component of reactive oxygen species (ROS), plays a crucial role in monitoring the occurrence and progression of diseases, including cancer. However, convenient and reliable analysis of H 2 O 2 levels released from cancer cells has remained particularly challenging. Herein, we proposed Pd single-atom loaded PdCoB alloy mesoporous nanospheres (Pd-PdCoB SAMNs) and 1,5-Diamino-4,8-dihydroxyanthraquinone-Cu metal-organic frameworks (DDA-Cu MOFs) for the reliable detection of the H 2 O 2 levels. In this approach, atomically dispersed Pd anchored on PdCoB mesoporous nanospheres (MNSs) with peroxidase-like catalytic activity, with the assistance of DDA-Cu MOFs nanobelts were then modified on the glassy carbon electrode (GCE) substrate to enhance its conductivity. Benefiting from the excellent electrochemical performances of Pd-PdCoB SAMNs and DDA-Cu MOFs, a detection limit of 0.74 μM and a linear detection range of 0.1 to 0.8 × 10 4 μM was achieved, and a high accuracy was reached in distinguishing the release of tumor cell lines from that of normal cells. Empowered by the intrinsic sensitivity and selectivity, the proposed approach will lead to the development of a universal platform for reliable small molecular. Download: Download high-res image (451KB) Download: Download full-size image
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2026
·
IF 19.7
Yutao Chen,Jihui Xiang,Jinmin Xie,Xinyu Wang,Zeyu Jiang,Yanfei Jian,Mudi Ma,Chi He
SO 2 exhibits opposite effects on C 3 H 8 oxidation over Pd/SiO 2 and Pt/SiO 2 . • O 2 concentration regulates sulfur species evolution and SO 2 tolerance. • Sulfate species block Pd active sites and induce Pd particle sintering over Pd/SiO 2 . • Pt-O-O-S structures on Pt/SiO 2 promote C 3 H 8 adsorption and C-H cleavage. The oxygen concentration in industrial C 3 H 8 -containing exhausts fluctuates significantly (from 0.5 to 18 vol%). However, the intrinsic effect of SO 2 on catalytic C 3 H 8 oxidation under diverse oxygen conditions is greatly overlooked, leading to a discrepancy in the SO 2 tolerance of developed catalyst between laboratory and real-world emission conditions. Herein, the influences of oxygen contents on sulfur species distribution and subsequent sulfur tolerance of typical Pd/SiO 2 and Pt/SiO 2 catalysts during C 3 H 8 oxidation were systematically explored. Experimental results reveal that the oxygen concentration dramatically affects the types and contents of sulfur species over catalysts. For Pd/SiO 2 , SO 2 tends to be converted into sulfate (SO 4 2- ) species to cover the Pd 0 active sites and causes Pd particle sintering, thereby inhibiting the C 3 H 8 adsorption and oxidation. In sharp contrast, sulfite (SO 3 2- ) species form on Pt/SiO 2 , leading to a novel Pt-O-O-S active interface that enriches the adjacent Pt site with electrons, promoting C 3 H 8 adsorption and C-H cleavage and further enhancing catalytic activity. As oxygen concentration decreases, the impact of SO 2 on catalytic performance becomes more pronounced. Under the oxygen-lean conditions, Pd particles sintering caused by SO 2 is the most severe at 1 vol% O 2 , causing an 80 °C temperature increasing in 90% C 3 H 8 conversion; however, the contents of SO 3 2- species and Pt-O-O-S structures on Pt/SiO 2 are elevated, facilitating C 3 H 8 adsorption and activation. Our findings enrich the understanding of SO 2 behavior under different industrial conditions, providing a theoretical basis for the design of SO 2 -tolerant catalyst in diverse application scenarios. Download: Download high-res image (178KB) Download: Download full-size image
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2025
·
IF 5.4
Huijin Chen,Huan Zhang,Xinyu Huang,Yakai Hao,Mingqiu Bao,Ruirui Yue,Jinbing Shu,Baoyang Lu
A qualified anode catalyst is the crucial component for one direct alcohol fuel cell. To facilitate the practical application of direct ethylene glycol fuel cells (DEGFCs), it holds significant importance to develop an anode catalyst with low cost, relatively high catalytic activity and reliable stability toward ethylene glycol oxidation reaction (EGOR). In this study, an in-situ polymerization method was employed to synthesize polydopamine (PDA)-functionalized reduced graphene oxide (rGO) as an efficient support for palladium nanoparticles (Pd NPs), ultimately resulting in the fabrication of a high performance Pd/PDA-rGO catalyst. Multiple physical characterization techniques confirm the consistent distribution of Pd NPs on the porous and fluffy PDA-rGO compound with open-textured structure. In the catalyst, rGO functions as a conductive component to boost the electronic conductivity of PDA and facilitates the formation of the wrinkled structure. Meanwhile, PDA granules can promote proton conductivity and prevent the aggregation of rGO. The unique morphological features of granular PDA and wrinkled rGO synergistically promote uniform Pd NPs distribution and improve their catalytic performance. The electrochemical evaluation of the EGOR was performed and it is found that the optimized Pd/PDA-rGO catalyst has remarkable mass activity and specific activity, which reached 3391.7 mA mg Pd −1 and 22.2 mA cm −2 . It also shows improved intrinsic activity, with a conversion frequency of 4.6 s −1 and excellent stability. The mass activity of Pd/PDA-rGO is about 8 times that of commercial Pd/C. This work establishes PDA-rGO as an ideal catalyst support and provides a strategy for designing advanced electrocatalysts.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2025
·
IF 5.4
Dexu Liu,Keyu Liu,Huifu Chi,Shan Gao,Shuangqing Fu,Wei Li,Honglei Zhang
Poly(3-hydroxybutyrate) (PHB) has emerged as a promising biodegradable polymer with extensive potential for diverse applications. When modified with chitosan (CS), PHB demonstrates enhanced metal-loading capabilities, significantly expanding its utility in environmental fields. In this study, a green heterobimetallic gold (Au) and palladium (Pd) catalyst (designated as Au/Pd@PHB-CS), was synthesized through a sequential coordination reduction process on the surface of the PHB-CS nanosphere. The resulting bimetallic nanoparticles on the nanosphere predominantly exhibit a particle size of approximately 4.0 ± 0.9 nm and expose a substantial number of highly active crystal planes. Catalysts possess adsorption capacities for three pollutants: congo red (CR), methylene blue (MB) and 4-nitrophenol (4-NP). Besides, catalysts with low bimetallic loading of Au (0.11 wt%) and Pd (0.11 wt%) show significant removal efficiencies for the three pollutants. Notably, in the degradation of CR, the catalyst exhibits complete reduction of CR with exceptionally fast reaction kinetics. Furthermore, the catalyst maintains a high catalytic activity (95%) after multiple cycles of utilization. Compared to monometallic Au or Pd catalysts, bimetallic catalysts exhibit significantly enhanced reaction activity due to the synergistic interaction between the two metal components. This improved catalytic performance underscores the potential of PHB-based materials as effective catalyst supports, broadening their research and application prospects in catalysis.
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PHYSICAL REVIEW B
·
2016
·Vol. 93
·期 21
·214510
·
IF 3.718
Kangkang Hu,Bo Gao,Qiucheng Ji,Yonghui Ma,Wei Li,Xuguang Xu,Hui Zhang,Gang Mu,Fuqiang Huang,Chuanbing Cai,Xiaoming Xie,Mianheng Jiang
We present a systematical study on the roles of interactions among electron correlation, electron-phonon coupling, and spin-orbit coupling in the isovalent Pd-substituted superconductor ${\mathrm{SrPt}}_{3}\mathrm{P}$. By using the solid state reaction method, the Pd element with the $4d$ orbital was successfully substituted in the strong spin-orbit coupling superconductors $\mathrm{Sr}{({\mathrm{Pt}}_{1\ensuremath{-}x}{\mathrm{Pd}}_{x})}_{3}\mathrm{P}$. As increasing the isovalent Pd concentrations without introducing any extra electron/hole carriers, the superconducting transition temperature ${T}_{c}$ decreases monotonously. In addition, combining the data of resistivity and specific heat, as well as electronic band structure calculations, we found that the electron correlation is enhanced while the electron-phonon coupling and the spin-orbit coupling are suppressed by Pd substitution. Our results may provide significant insights in the natures of the interplay among the electron correlation, electron-phonon coupling, and spin-orbit coupling in superconductivity, and may also pave a route for understanding the mechanism of superconductivity in heavily $5d$-based superconductors.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2023
·
IF 5.2
Zhenzhen Tang,Derong Xu,Hongyu Chen,Si Tang,Chunlin He,Shunyan Ning,Min Li,Guoyuan Yuan,Shuangkou Chen,Jian Feng
Metal-organic frameworks are recognized as a new kind of potential adsorbent for wastewater treatment because of their tunable pore size, high surface area and modifiable functionality. In this work, 2,6-diaminopyridine functionalized UiO-66-NH 2 (UiO-66-DAP) was synthesized by a post-modification strategy and was applied to the adsorption of Pd(Ⅱ) from aqueous solution. The aminopyridine structure on UiO-66-DAP greatly improved the adsorption performance for Pd(II), with an adsorption capacity of 190.95 mg/g. The adsorption process of Pd(Ⅱ) on UiO-66-DAP was consistent with the pseudo-second-order kinetic model and the Langmuir adsorption isotherm . Thermodynamic studies confirmed that the adsorption process was endothermic and spontaneous. Regeneration studies showed that UiO-66-DAP was stable and recyclable. Moreover, UiO-66-DAP could maintain high selectivity to Pd(Ⅱ) even in a wastewater containing multiple interfering metal ions. According to the results of Fourier transform infrared spectroscopy (FT-IR), scanning electron microscopy (SEM), energy-dispersive X-ray spectroscopy (EDS), X-ray photoelectron spectroscopy (XPS), zeta potential , comparative experiments and DFT calculations, the chelation and electrostatic attraction between Pd(Ⅱ) and the aminopyridine structural unit are the dominant mechanisms. Using UiO-66-DAP as an adsorbent, this study provides a promising way for the separation of palladium form wastewater.
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ChemCatChem
·
2023
·Vol. 15
·期 7
·e202300194
·
IF 4.5
Tao Li,Mengling Dong,Jiacheng Xu,Tiantian Zhang,Yan Sun,Ning Li,Zuliang Wu,Jing Li,Erhao Gao,Jiali Zhu,Shuiliang Yao,Yong Huang
Graphical CeO 2 /γ-Al 2 O 3 , Pd/CeO 2 , and Pd/CeO 2 /γ-Al 2 O 3 were used for catalyzing low-concentration CH 4 oxidation . γ-Al 2 O 3 can efficiently promote CH 4 oxidation on Pd/CeO 2 and the formation of bicarbonate that is easily gasified to CO 2 . CeO 2 /γ-Al 2 O 3 , Pd/CeO 2 , and Pd/CeO 2 /γ-Al 2 O 3 were used for catalyzing low-concentration CH 4 oxidation. It was found that nano-sized Pd could obviously promote CH 4 oxidation on CeO 2 /γ-Al 2 O 3 . The interaction between Pd and CeO 2 on γ-Al 2 O 3 resulted in higher ratios of Ce 3+ /(Ce 3+ +Ce 4+ ), Pd 2+ /(Pd 2+ +Pd δ+ ), and O ads /(O ads +O latt ), those benefited the formation of more oxygen vacancies and surface reactive oxygen species for CH 4 oxidation. γ-Al 2 O 3 not only supplied a high surface area and enhanced Pd/CeO 2 dispersion on γ-Al 2 O 3 , but also simulated the formation of bicarbonate, where bicarbonate is easier to gasify to CO 2 than bidentate carbonate that formed on Pd/CeO 2 . Operando diffuse reflectance infrared Fourier transform spectroscopy-mass spectrometer analysis results showed that CH 4 oxidation could occur at a temperature as low as 180 °C due to the reaction with surface reactive OH, this reaction was also accompanied by the formation of bicarbonate. The mechanism of CH 4 oxidation promoted by bicarbonate formation on γ-Al 2 O 3 was proposed.
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Cell Death & Disease
·
2023
·Vol. 14
·期 2
·1-13
·
IF 9
Liu Nian,Zhang Jianglin,Yan Mingjie,Chen Lihui,Wu Jie,Tao Qian,Yan Bei,Chen Xiang,Peng Cong
Patients with advanced melanoma have shown an improved outlook after anti-PD1 therapy, but the low response rate restricts clinical benefit; therefore, enhancing anti-PD1 therapeutic efficacy remains a major challenge. Here, our findings showed a significantly increased abundance of α-KG in healthy controls, anti-PD1-sensitive melanoma-bearing mice, and anti-PD1-sensitive melanoma patients; moreover, supplementation with α-KG enhanced the efficacy of anti-PD1 immunotherapy and increased PD-L1 expression in melanoma tumors via STAT1/3. We also found that supplementation with α-KG significantly increased the activity of the methylcytosine dioxygenases TET2/3, which led to an increased 5-hydroxymethylcytosine (5-hmC) level in the PD-L1 promoter. As a consequence, STAT1/3 binding to the PD-L1 promoter was stabilized to upregulate PD-L1 expression. Importantly, single-cell sequencing of preclinical samples and analysis of clinical data revealed that TET2/3-STAT1/3-CD274 signaling was associated with sensitivity to anti-PD1 treatment in melanoma. Taken together, our results provide novel insight into α-KG’s function in anti-PD1 treatment of melanoma and suggest supplementation with α-KG as a novel promising strategy to improve the efficacy of anti-PD1 therapy.
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Xuewu Deng,Xiaobing Zheng,Feifei Jia,Cuiyao Cao,Haolei Song,Yanjun Jiang,Yunting Liu,Guanhua Liu,Shijie Li,Lihui Wang
The selective oxyfunctionalization of C-H and C C bonds is highly important and catalyzed by unspecific peroxygenases (UPOs) which suffer from inactivation by hydrogen peroxide (H 2 O 2 ). Herein, photo-enzyme integrated catalysts were constructed by immobilizing Aae UPO as cross-linked enzyme aggregates (CLEAs) in Pd-loaded three-dimensional ordered macroporous titania (3DOM TiO 2 ) with in situ photocatalytic H 2 O 2 production. The prepared Aae UPO@3DOM TiO 2 -Pd obtained higher catalytic efficiency compared with CLEAs- Aae UPO. The conversion of ethylbenzene to (R) -1-phenethyl alcohol was significantly improved, reaching 99 % compared with free enzyme (38 %) and CLEAs- Aae UPO (49 %), with ee value of > 99 %. Aae UPO@3DOM TiO 2 -Pd exhibited good stability and reusability attributed to the protection of macropores and in situ H 2 O 2 production. By using the designed 3DOM platform for photocatalysis and enzyme immobilization, the in situ photocatalytic generation of H 2 O 2 was highly efficient, and the monodisperse CLEAs- Aae UPO in the macropores facilitated the contact of substrate and enzyme, thus obtaining excellent photo-enzyme coupled catalysis.
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高影响因子
Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Lulu Zhang,Long Jiang,Yaojie Liu,Zongjiang Yu,Ximin Chen,Xiaomeng Su,Mo Xian,Weizhi Sun,Chao Xu
Currently searching for effective noble metal separation material is generally blind and time-consuming. Although theoretical calculation has been widely applied to explain the adsorption mechanism, the quantitative coordination effect between ligand and metal remains to be explored especially in the material screening stage. In this study, Pearson’s theory and Koopmans' theory were used to calculate the electron transfer ratio (ΔN) from different ligands containing N, S, and O to PdCl 2 . The quantitative evaluation contributed to the design of efficient ligands including EA (ΔN =0.5929), DB (ΔN =0.5483), and AT (ΔN =0.4885). And the corresponding polystyrene materials CMPS-EA, CMPS-AT, CMPS-DB were successfully synthesized via chemical modification. According to the adsorption experiment, the per mmol of ligand adsorption capacity from CMPS-EA, CMPS-DB and CMPS-AT for Pd(II) were 0.67 mmol/mmol, 0.17 mmol/mmol and 0.11 mmol/mmol, respectively, exhibiting a positive correlation with the results of ΔN. Moreover, CMPS-EA could efficiently remove 98.01% Pd(II) in the presence of multiple competing metal ions with five times concentration higher than Pd(II). In column study, the breakthrough point (C t /C 0 =0.05) for CMPS-EA was 666–676 BV in 1 mmol/L Pd(II) solution and up to 95% desorption efficiency within 50 BV. The adsorption differences and mechanism of CMPS-EA, CMPS-AT and CMPS-DB were further investigated by FTIR, XPS, ESP, and NBO.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2022
·
IF 7.139
Zuqin Duan,Qian Lei,Wenhui Wu,Honglin Chen
Hydrogen release from formic acid is a significant energy supply route. However, the current catalysts suffer from low catalytic efficiency and stability. Herein, a porous N-doped carbon material with high N content (16.87%) and a large surface area (1544 m 2 ·g −1 ) were designed using a 2-dimensional metal-organic framework and etching agent potassium chloride . Due to its high N content and large surface area, ultrafine Pd particles are uniformly distributed on the porous N-doped carbon support, which effectively enhances excellent reactivity and enables a TOF value of 2365 h −1 under additive-free conditions. The research also revealed that the strong interaction between Pd particles and pyridinic-N species can significantly slow metal agglomeration. Hence, the Pd/NC ZIF-L (KCl) displayed good activity even after 10 cycling experiments, and it is a particularly competitive catalyst for hydrogen release from formic acid.
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