ADVANCED MATERIALS
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2025
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IF 26.8
Xiejun Zhao,Xiangchuan Qin,Ruizhe Wang,Yawen Wang,Yinli He,Yuchen Wang,Kefeng Li,Peipei Zhang,Chen Yang,Menghan Wang,Yingtong Dong,Xue Shi,Jia Ma,Jiye Zhang,Xiaojiao Li
Inefficient priming, poor recruitment, and inadequate reinvigoration of T cells challenges the therapy of PD-L1-resistant tumors. Herein, a pH-responsive charge-reversal nanoplatform integrating coactivator-associated arginine methyltransferase 1 (CARM1) inhibitor (iCARM1) and poliovirus receptor siRNA (siPVR) is developed. Upon tumor penetration, iCARM1 released in tumor cells facilitates T cell priming by epigenetically activating cyclic GMP-AMP synthase (cGAS)-stimulator of interferon genes (STING) signaling-mediated dendritic cell maturation. Meanwhile, in T cells, iCARM1 facilitates their recruitment by upregulating CXC-chemokine receptor 3 (CXCR3) expression. The released siPVR silences pvr to reinvigorate T cells. This epigenetic nanoagonist induces a robust immune response, dramatically suppresses tumor growth, metastasis, and relapse, and confers durable protection against secondary tumor challenge. Multiple PD-L1-resistant models demonstrate the broad applicability of this strategy. This study thus represents an innovative approach for facilitating multilevel T cell responses to combat PD-L1-resistant tumors.
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CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Xiangyu Jia,Kai Yuan,Guofu Wang,Shanhui Zhu,Mei Dong,Jiamin Wang,Xiaoming Li,Weibin Fan
Selective reduction of 5-hydroxymethylfurfural (HMF) to valuable 2,5-bis(hydroxymethyl)tetrahydrofuran (BHMTHF) remains a significant challenge under mild conditions. The synergistic effect between metal single atoms (SAs) and nanoparticles (NPs) can greatly enhance catalytic activity. Here, a high-performance Pd SAs catalyst supported on N-doped carbon (PdSAs/NC) was developed from Pd@UiO-66-NH 2 . It was found that partial Pd SAs were spontaneously restructured into Pd NPs during the reaction. Our catalyst exhibited 100 % conversion of HMF and 98 % selectivity towards BHMTHF at temperature as low as 0 °C. In situ FTIR spectra results and density functional theory calculations indicate that Pd SAs contribute to the C = O activation, while Pd NPs facilitated the H 2 dissociation into H* atoms, resulting in synergistic catalytic activity between Pd SAs and Pd NPs.
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Journal of Materials Chemistry A
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2025
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IF 9.5
Mingjing Ma,Huanhuan Yu,Baolin Zhu,Wenjun Zheng,Shoumin Zhang
The design of efficient catalysts with atom clusters (ACs) and single atoms (SAs) as active sites for water splitting presents an effective approach for improving bifunctional electrocatalytic performance by synergistically promoting electron transport and proton transfer kinetics. In this work, a series of Fe2O3-supported noble metal catalysts (M = Ru, Rh, Pd, Ag) incorporating both ACs and SAs sites were developed, with detailed characterization identifying Ru ACs as the primary active centers. The designed-interfacial M-O-Fe bonds play a critical role in charge redistribution, subsequently enhancing electron and proton transfer kinetics. The resulting heterostructure optimizes both the electronic environment and active site accessibility, yielding exceptional electrocatalytic performance. Further density functional theory calculations demonstrate that the incorporation of Ru species leads to increased filling of antibonding orbitals and modulation of the d-band center, subsequently reducing the energy barrier of the rate-determining steps to −0.267 eV for HER and 1.522 eV for OER, respectively. Consequently, the representative Ru/Fe2O3 with Ru content of 1.1 wt.% achieves an OER overpotential of 189 mV and a HER overpotential of 21 mV at a current density of 10 mA cm−2. This study highlights a novel approach to the design of advanced bifunctional electrocatalysts by engineering interfacial bridge bonds.
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Science Advances
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2025
·Vol. 11
·期 29
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IF 12.5
Zhenyu Li,Kunhong Jiang,Yue Yang,Yijing Pian,Huizhen Liu,Zexuan Zheng,Xiyang Wang,Subhajit Jana,Jiefei Li,Zhuoyuan Ma,Xiaoyun Qiao,Xiaoxin Zou,Xuelu Ma,Bin Zhang,Haibin Chu,Yimin A. Wu
Glycerol oxidation reaction (GOR) represents an economical pathway for transforming renewable feedstock to value-added chemicals. However, the inertness of C(sp 3 )─H bonds of glycerol and intermediates results in the high energy barrier of the dehydrogenation step, relating to poor product selectivity at high glycerol conversion. Here, a carbon nanotube–supported PdBO x @Pd heterostructure catalyst (PdBO x @Pd/CNTs) was synthesized in which in situ–exsoluted PdBO x clusters covalently covered Pd nanoparticles, thus yielding strong electronic interaction between Pd nanoparticles and PdBO x clusters. The strong electronic interaction in PdBO x @Pd/CNTs induces the hybridization between Pd(d), B(s, p), and O(s, p) atom orbits, optimizing the adsorption of reactants and intermediates, thus enhancing the activity for the GOR. The density functional theory calculation result reveals that the strong electronic interaction in PdBO x @Pd/CNTs facilitates the hydrogen transfer in the primary C─H bond of the CH 2 OHCHOHCH 2 O* intermediate, thus reducing the energy barrier of the rate-determining step and improving glyceric acid selectivity toward the GOR.
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ACS Applied Materials & Interfaces
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2025
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IF 8.2
Zhen-Ming Lu,Zi-Wen Qiu,Yan-Mei Li,Ke-Yan Zhang,Ye-Yang Wu,Ni Yan,Hong Cheng
Breast cancer cells are characterized by heightened autophagy, which impairs tumor-associated antigen presentation and represents a significant barrier to the antitumor immunity. In this study, a PD-L1-targeting autophagy modulator (PFC@CQ) is fabricated to activate the photoimmunotherapy against breast cancer. Specifically, the hydrophobic photosensitizer protoporphyrin IX (PpIX) is covalently linked to the hydrophobic peptide FFVLK and a PD-L1-targeting peptide sequence CLQKTPKQC, resulting in the formation of an amphiphilic photosensitizer-peptide conjugate (PpIX-FFVLK-CLQKTPKQC, called PFC), which is capable of encapsulating the autophagy inhibitor chloroquine (CQ). PFC@CQ can not only facilitate the targeted drug codelivery to PD-L1-overexpressing breast cancer cells, but also effectively disrupt their immune evasion by blocking PD-1/PD-L1 pathway. Upon light irradiation, the photodynamic therapy (PDT) of PFC@CQ induces tumor cell destruction and immunogenic cell death (ICD), causing the release of damage-associated molecular patterns (DAMPs). Simultaneously, PFC@CQ can inhibit autophagy pathway to mediate the upregulation of MHC-I, thereby enhancing antigen presentation. This cascade immunomodulation promotes the dendritic cell maturation and CD8+ T cell activation, leading to a synergistic suppression of both primary and metastatic tumors. This work introduces an innovative autophagy modulation strategy with potent immunomodulatory capability, demonstrating a potential to trigger systemic antitumor immune responses through local treatment.
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ACS Applied Materials & Interfaces
·
2024
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IF 8.3
Xianbin Xu,Difei Xiao,Yugang Gao,Wenbo Li,Miaomiao Gao,Shuang Zhao,Zeyan Wang,Zhaoke Zheng,Peng Wang,Hefeng Cheng,Yuanyuan Liu,Ying Dai,Baibiao Huang
Electrocatalytic CO2 reduction reaction (CO2RR) to high value-added products, such as ethylene (C2H4), offers a promising approach to achieve carbon neutrality. Although recent studies have reported that a tandem catalyst (for example, Cu–Ag systems) exhibits advantage in C2H4 production, its practical application is largely inhibited by the following: (1) a traditional tandem catalyst cannot effectively stabilize the *CO intermediate, resulting in sluggish C–C coupling, and (2) inadequate H2O activation ability hinders the hydrogenation of intermediates. To break through the above bottleneck, herein, palladium (Pd) was introduced into Cu2O–Ag, a typical conventional tandem catalyst, to construct a Cu2O–Pd–Ag ternary catalyst. Extensive experiment and density functional theory calculation prove that Pd can efficiently stabilize the *CO intermediate and promote the H2O activation, which contributes to the C–C coupling and intermediate hydrogenation, the key steps in the conversion of CO2 to C2H4. Beneficial to the efficient synergy of Cu2O, Pd, and Ag, the optimal Cu2O–Pd–Ag ternary catalyst achieves CO2RR toward C2H4 with a faradaic efficiency of 63.2% at −1.2 VRHE, which is higher than that achieved by Cu2O–Ag and most of other reported catalysts. This work is a fruitful exploration of a rare ternary catalyst, providing a new route for constructing an efficient CO2RR electrocatalyst.
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IMMUNITY
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2024
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IF 25.5
Jiping Sun,Youqin Zhang,Qingbing Zhang,Lin Hu,Linfeng Zhao,Hongdong Wang,Yue Yuan,Hongshen Niu,Dongdi Wang,Huasheng Zhang,Jianyue Liu,Xujiao Feng,Xiaohui Su,Ju Qiu,Jing Sun,Heping Xu,Catherine Zhang,Kathleen Wang,Yan Bi,Edgar G. Engleman,Lei Shen
Adipose tissue group 2 innate lymphoid cells (ILC2s) help maintain metabolic homeostasis by sustaining type 2 immunity and promoting adipose beiging. Although impairment of the ILC2 compartment contributes to obesity-associated insulin resistance, the underlying mechanisms have not been elucidated. Here, we found that ILC2s in obese mice and humans exhibited impaired liver kinase B1 (LKB1) activation. Genetic ablation of LKB1 disrupted ILC2 mitochondrial metabolism and suppressed ILC2 responses, resulting in exacerbated insulin resistance. Mechanistically, LKB1 deficiency induced aberrant PD-1 expression through activation of NFAT, which in turn enhanced mitophagy by suppressing Bcl-xL expression. Blockade of PD-1 restored the normal functions of ILC2s and reversed obesity-induced insulin resistance in mice. Collectively, these data present the LKB1-PD-1 axis as a promising therapeutic target for the treatment of metabolic disease.
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Chemical Science
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2025
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IF 7.4
Yiyan Yin,Xiaorong Wang,Xiyang Ge,Xiaotong Shen,Xiaomin Liu,Xiang Li,Jin Ouyang,Na Na
The palladium-catalyzed Suzuki-Miyaura cross-coupling (SMCC) reaction is an essential technique for C-C bond formation. It is considered to occur through two distinct pathways involving homogeneous and heterogeneous mechanisms. However, there is still debate about these mechanisms given the lack of direct structural evidence in both spatial and temporal terms, especially regarding the conversion of active Pd species. In this study, the Pd single-atom catalyst (Pd SAC) SMCC reaction was monitored in real-time using ambient mass spectrometry (AMS) to study conversions of Pd species both on the catalyst surface and in the liquid phase. This revealed a leaching-oxidizing-landing paths as a contributor to the heterogeneous process which involves heterogeneous oxidative addition, Pd leaching along with transmetallation (rather than oxidative addition), and subsequent oxidation-landing back onto the catalyst surface. The leaching-oxidizing-landing mechanism of Pd active sites during Pd SAC-catalyzed SMCC reaction provides an explanation for the Pd migration on the catalyst surface. A crucial role of molecular oxygen during SMCC reaction was revealed and attributed to the re-deposition of active Pd species by coordinating with the catalyst support. Overall, the leaching-oxidizing-landing mechanism of the SMCC reaction has been revealed and it not only provides insights into mechanism studies and catalyst designs, but it enlarges AMS applications.
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BIOMATERIALS
·
2025
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IF 12.9
Zhanxue Xu,Xinrui Yang,Xingyu Lu,Dandan Su,Yidan Wang,Huixing Wu,Zhenhua Zhang,Changrui Long,Liqian Su,Yanyu Wang,Hongbo Chen,Shijian Xiang,Benjie Zhou
Combination therapies for melanoma face challenges due to asynchronous drug delivery and associated toxicity, underscoring the need for advanced delivery systems. While immune checkpoint inhibitors (ICIs) enhance T cell activity, optimal cytotoxic responses require efficient antigen presentation by mature dendritic cells (DCs), which are often functionally impaired in the tumor microenvironment. Thus, effective treatment requires coordinated T cell activation, DC-mediated priming, and direct tumor suppression. Herein, wild Glycyrrhiza uralensis Fisch roots-derived nanovesicles (GC NV) are demonstrated to be effective inhibitors of melanoma proliferation. The vesicles exert this activity through the intracellular delivery of encapsulated miRNA (miR2916) and bioactive molecules (isoliquiritigenin), with this capacity for intracellular delivery extending to the STING agonist DMXAA. We also demonstrate how chemical modification can be used to install PD-L1 antibodies on the membrane surface of these GC NV, imbuing these vesicles with selectivity for tumor cells. Combining DMXAA encapsulation with surface-displayed PD-L1 antibodies creates vesicles (GP@DMX NV) that both promote DCs maturation and elicit CD8 + T cell response. Our multifunctional GP@DMX NV reverse the immunosuppressive microenvironment of melanoma and significantly enhance the immunotherapeutic potential of immune checkpoints.
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Nature Communications
·
2022
·Vol. 13
·期 1
·1-10
·
IF 17.694
Yang Yang,Zhu Xiaojuan,Wang Lili,Lang Junyu,Yao Guohua,Qin Tian,Ren Zhouhong,Chen Liwei,Liu Xi,Li Wei,Wan Ying
Pd catalysts are widely used in alkynol semi-hydrogenation. However, due to the existence of scaling relationships of adsorption energies between the key adsorbed species, the increase in conversion is frequently accompanied by side reactions, thereby reducing the selectivity to alkenols. We report that the simultaneous increase in alkenol selectivity and alkynol conversion is achieved by manipulating interstitial atoms including B, P, C, S and N in Pd catalysts. A negative linear relationship is observed between the activation entropies of 2-methyl-3-butyn-2-ol and 2-methyl-3-buten-2-ol which is highly related to the filling of d -orbital of Pd catalysts by the modification of p -block elements. A catalyst co-modified by B and C atoms has the maximum d charge of Pd that achieves a 17-fold increase in the turn-over frequency values compared to the Lindlar catalysts in the semi-hydrogenation of 2-methyl-3-butyn-2-ol. When the conversion is close to 100%, the selectivity can be as high as 95%.
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INORGANIC CHEMISTRY
·
2025
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IF 4.7
Junxiang Lu,Yuting Liu,Shasha Zhang,Juhong Nie,Bing Tang,Jia Guan,Jian Zhang
Regulating the strength of coordination bonds plays an important role in synergizing the activity and stability of single-atom catalysts (SACs) but is often limited due to coordination atoms from the inorganic carrier lattice being tough to modify. It is fascinating yet rarely explored to immobilize organic molecules on lattice atoms for modulating the character of coordination bonds. Herein, a valid inorganic–organic coupling strategy is developed to enhance Pd–O coordination bonds within Pd-SAC for reconciling activity and stability. Nickel hydroxide enriched with Ni2+ vacancies is utilized to bind Pd centers, and dimethylglyoxime (DMG) bonds with its OH groups by H2 reduction, forming a Pd–O-DMG structure. Compared with the pristine Pd–O structure, whose activity descends greatly during the recycling process, the Pd–O-DMG structure makes the activity unchanged after 6 used times for the Suzuki–Miyaura reaction. The Pd-SAC has mild and economic reaction conditions (at 70 °C under air in ethanol without excess base) and good substrate tolerance. Further theoretical calculations show that coupled DMG induces hydrogen bonds on O atoms of the oxazole around Pd centers and thus strengthens Pd–O coordination bonds to exhibit good stability and activity.
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International Journal of Nanomedicine
·
2025
·
IF 6.5
Li Gao,Li-Hua Yang,Fang-Cheng Jiang,Wang-Yang Ye,Xin Chen,Zhao-Ji Liu,Rong-Quan He,Wan-Ying Huang,Zhen-Bo Feng,Jin-Liang Kong,Ze-Feng Lai,Gang Chen
Background Although immune checkpoint blocking (ICB) therapeutic agents have significantly improved the survival for many cancer patients, the efficacy of ICB therapy for non-small cell lung cancer (NSCLC) patients remains limited. Combining ICB therapy with other strategies that is able to stimulate tumor immunogenicity or increase infiltration of T cells aroused great concern in cancer therapy.Results Herein, we constructed a kind of AuNP@NH2-PEG-SH/PD-L1 siRNA nanoparticle complex which showed prominent photothermal therapeutic (PTT) effects triggered by NIR laser and could efficiently deliver PD-L1 siRNA into NSCLC cells (knock-down efficiency were 75.8% and 83% in HCC827 and A549 cells). During the process of photothermal stimulation, discrepancies in heat shock protein expression were observed in NSCLC cells. Knocking down PD-L1 expression in NSCLC cells such as A549 and HCC827 cells activated the co-culturing Jurkat cells and enhanced their tumor-killing effect in vitro (cell inhibition rate was 62.65% for HCC827 cells and 57.03% for A549 cells). The gold nanoparticle complexes exhibited remarkable PTT effect for the engrafted NSCLC cells in zebrafish larvas. Furthermore, the nano complexes could promote the activation of the xenografted human peripheral blood mononuclear cells (PBMCs) and enhance the killing of the NSCLC cells in the larvas.Conclusion It is well known that gold nanoparticle is one of the several metal nanoparticles approved for clinical trial by American FDA. This work has demonstrated the outstanding PTT and immunotherapeutic effects of gold nanoparticle complexes on NSCLC, indicating great potential in clinical regiment of lung cancers.
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