JOURNAL OF CONTROLLED RELEASE
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2022
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IF 11.467
Junlin Li,Yue Yan,Ping Zhang,Junzhou Ding,Yuan Huang,Yun Jin,Lian Li
Immune checkpoint blockade (ICB) can elicit anti-cancer response against tumors growing at normal organs while sparing adjacent tissues. However, many orthotopic tumors respond poorly to ICB therapy due to the lack of pre-existing immune effector cells. Here, we describe a vaccine strategy that induces protective immunity and benefits ICB therapy. An injectable hydrogel platform that forms scaffold subcutaneously was applied to deliver autologous cancer cells undergoing oncolysis (ACCO) as immunogenic antigen source and toll-like receptor 9 agonists (CpG) as additional adjuvant. When administered as a prophylactic, the hydrogel-based vaccine, denoted as (ACCO+CpG)@Gel, successfully built a durable and tumor antigen-specific immune memory against subsequent challenges with orthotopic engraftment of autologous tumors including melanoma , colon carcinoma , and lung carcinoma . Although the vaccination did not completely prevent tumor occurrence, tumors orthotopically established in vaccinated mice acquired significant enhancement in tumor-infiltrating CD8+ T cells and intratumoral PD-L1 expression, which ameliorated the immune status and rendered the originally irresponsive tumors responsible to anti-PD-L1 therapy. Further treatment with PD-L1 blockade therapy efficiently delayed the tumor growth and prolonged the survival of these orthotopic cancer models. Thus, without the need for precisely delivering immunoactivatory agents to tumor or locally remodeling tumor microenvironment , “priming” intractable or inaccessible tumors for subsequent ICB therapy could be achieved by prophylactic vaccination with (ACCO+CpG)@Gel. These findings highlighted (ACCO+CpG)@Gel as a generalized framework of protective vaccine strategy that could be broadly applicable to potentiate ICB therapy against multiple types of orthotopic tumors growing in different regions.
研究领域:
肿瘤学
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免疫治疗
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生物医学工程
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癌症免疫学
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PubMed
高影响因子
ENERGY & FUELS
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2025
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IF 5.3
Qiulin Ye,Dongdong Wang,Jiabao Lv,Minghui Tang,Angjian Wu,Yaqi Peng,Shengyong Lu
The electrocatalytic CO2 conversion offers a sustainable pathway for generating ecofriendly chemicals and fuels while simultaneously enabling the storage of intermittent renewable energy. Herein, CuPd bimetallic catalysts were specifically designed through displacement reaction, with a magnetron sputtering Cu film as a substrate. The optimized CuPd catalyst achieved an ethylene Faradaic efficiency (FE) of 51.07% and a C2+ FE of 82.18% at a 200 mA/cm2 current density. In situ Raman spectroscopy indicates that the CuPd electrode exhibited a high local surface pH during the CO2 reduction reaction, which was favorable for C–C coupling. The observation of the *OCCOH intermediate by in situ FTIR, combined with density functional theory calculations, confirms that the CuPd surface promotes C–C coupling instead of direct hydrogenation. This mechanistic insight explains why the addition of Pd enhances the selectivity for C2+ products.
研究领域:
电催化
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材料科学
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可持续能源
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表面化学
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二氧化碳利用
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Nanomaterials
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2025
·Vol. 16
·期 1
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IF 4.3
Yu Zhang,Ying Xin,Lizheng Tang,Shihao Cui,Hongling Duan,Qingshan Zhao
The selective hydrogenation of phenol to cyclohexanone is a pivotal reaction for producing nylon precursors. Conventional Pd/C catalysts, however, suffer from weak metal–support interactions, leading to size heterogeneity and agglomeration of Pd nanoparticles, which degrades their activity and stability. Herein, we report a facile argon plasma treatment to engineer rich defects on an activated carbon (AC) support, resulting in a highly dispersed and stable catalyst (denoted as PL-Pd@ACAr). Characterization results indicate that the abundant carbon defects in PL-Pd@ACArenhance the anchoring of Pd precursors, ensure the uniform dispersion of Pd nanoparticles, and effectively modulate their electronic structure. Consequently, the plasma-enabled PL-Pd@ACArcatalyst achieves 99.9% phenol conversion with 97% selectivity to cyclohexanone at a mild temperature of 70 °C and maintains exceptional stability over six consecutive cycles. This work provides a robust and efficient strategy for the surface engineering of carbon supports to design high-performance hydrogenation catalysts.
研究领域:
催化化学
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材料科学
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化学工程
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绿色化学
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PubMed
高影响因子
Advanced Materials Interfaces
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2026
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IF 4.5
Chunmin Jia,Yimin Lei,Hong Xu,Xin Meng,Yuxiang Wei,Peixian Li,Xiaohua Ma,Yue Hao,Xiaohui Jia
Programmed death-1 (PD-1) is a key biomarker for monitoring therapeutic response and resistance in non-small cell lung cancer (NSCLC) immunotherapy. Achieving highly sensitive, real-time detection of PD-1 is crucial for early prediction of treatment resistance and disease recurrence. However, current methods such as ELISA suffer from limitations in sensitivity, speed, and cost. To address these challenges, we develop a label-free biosensor based on semiconducting single-walled carbon nanotube field-effect transistors (CNT-FETs). The sensing interface is designed by wrapping s-SWCNTs with poly[9-(1-octylnonyl)-9H-carbazole] (PCz), enabling immobilization of anti-PD-1 antibodies via cation-π interactions. XPS analysis confirms antibody immobilization via reversible binding energy shifts in C 1s and N 1s spectra upon salt treatment, consistent with cation-π interactions, further validated by NaCl and imidazole competition assays. Using this strategy, the sensor achieves a detection limit of 8.39 fg/mL for murine PD-1—three orders of magnitude lower than ELISA, along with good specificity and favorable regeneration capability. In human serum, it shows promising performance, with 12 out of 14 NSCLC patient samples (85.7%) exhibiting good linear correlation. With rapid response, low cost, and simple operation, this platform offers a reliable strategy for point-of-care PD-1 monitoring during NSCLC immunotherapy.
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Materials Today Bio
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2026
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IF 11
Xueping Luo,Yixin Liu,Guangmiao Chen,Xinrui Ma,Pingping Xu,Yutong Li,Longyu Zheng,Rongrong Zheng,Youqin Xu,Shiying Li,Linping Zhao
Ferroptosis, a form of regulated cell death that is iron-dependent and driven by the accumulation of lipid peroxides (LPO), has emerged as a promising avenue for enhancing tumor immunogenicity and augmenting immune checkpoint blockade (ICB) efficacy. In this study, we demonstrated that dBET57, a BRD4-targeting PROTAC, potently suppresses the expression of GPX4, the master negative regulator of ferroptosis, thereby triggering ferroptotic cell death, while concurrently downregulating PD-L1 to reverse immune evasion. Based on this, we developed a self-assembled nano-PROTAC platform, termed dBET@TF, designed to amplify ferroptosis and potentiate colorectal cancer immunotherapy. Specifically, dBET@TF was constructed via self-assembly of dBET57, tannic acid, and Fe 3+ , which endowed the formulation with acid-responsive drug release capability and significantly improved its intracellular delivery efficiency. Mechanistically, dBET@TF promoted ferroptosis through iron accumulation and GPX4 depletion, triggering robust immunogenic cell death (ICD). Concurrently, BRD4 degradation mediated by dBET@TF durably suppressed PD-L1 expression, reprogramming the tumor microenvironment to foster enhanced immune activation, characterized by increased infiltration of natural killer (NK) cells and cytotoxic T lymphocytes (CTLs). As a result, dBET@TF significantly potentiated the therapeutic response to αPD-1 in both primary tumor and experimental lung metastasis models. Overall, this work establishes a novel PROTAC-based therapeutic strategy that leverages BRD4 degradation to amplify ferroptosis and remodel antitumor immunity, offering a promising approach to potentiate colorectal cancer immunotherapy.
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ACS Applied Nano Materials
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2026
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IF 5.8
Xinru Wang,Lei Jin,Wenqian Li,Yu-Shi He,Jinglin Mu,Weimin Zhang
Electrocatalytic hydrogenation dechlorination (EHDC) has emerged as a promising and environmentally benign strategy for the degradation of chlorinated phenols (CPs), owing to its green process characteristics and the absence of hazardous byproducts. Achieving high EHDC efficiency necessitates both a highly active electrocatalyst and optimized reaction conditions. In this work, we fabricated a Pd/Co3O4 electrode, comprising ultralow-loading Pd nanoparticles (0.011 mg Pd cm–2) supported on a Co3O4 nanoarray grown on carbon fiber paper (CFP), for EHDC applications. The well-defined array structure facilitates uniform potential and current density distribution while also expanding the number of electroactive sites. Electrochemical and theoretical analyses reveal that abundant oxygen vacancies (OVs) in Co3O4 induce a spatial charge redistribution in the Pd/Co3O4 heterostructure, thereby strengthening the metal-support interaction (SMSI). This optimization of geometric and electronic properties significantly enhances both hydrogen evolution capability and EHDC performance. Under optimized operational parameters, including pH, substrate concentration, and applied potential, the Pd/Co3O4/CFP electrode achieves nearly complete degradation (close to 100%) of 10 mg·L–1 4-chlorophenol (4-CP) within 180 min at a cathodic potential of −0.8 V vs Ag/AgCl, with phenol (P) as the main product. The mass activity (MA) for 4-CP dechlorination reaches 1.0289 min–1 mg–1. Density functional theory (DFT) calculations further illustrate that the underlying oxygen vacancy rich Co3O4 modulates the electronic structure of Pd, boosting hydrogenation capacity and EHDC efficiency. These findings underscore the great potential of the Pd/Co3O4/CFP electrode as an efficient and practical electrocatalyst for EHDC processes.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2026
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IF 9.1
Ruiying Xie,Feng Zhang,Guishan Hu,Mengzhen Chen,Huixian Wang,Xiaoquan Feng,Xuerui Wang,Yatao Zhang,Meixia Shan
The widespread presence of toxic nitroaromatic compounds in industrial effluents demands advanced remediation strategies. Catalytic reduction is highly effective, while the practical application of powdered catalysts is limited by challenges in recovery and reuse. To overcome this issue, macroscopic Pd@NH 2 -MIL-101/AOPIM-1 porous composite beads were fabricated via a phase inversion method, combining the high surface area of NH 2 -MIL-101 with the excellent processability of amidoxime-functionalized polymers of intrinsic microporosity (AOPIM-1). The incorporation of NH 2 -MIL-101 enriches the composite with amino functional groups, thereby enhancing the adsorption and local enrichment of reactants. Furthermore, these nitrogen-rich sites provide robust anchoring points for the uniform dispersion of Pd nanoparticles, collectively boosting catalytic activity and structural stability. The beads exhibited outstanding catalytic activity for the reduction of nitroaromatics, achieving 99% conversion of 4-nitrophenol (4-NP) within 5 min. The catalyst also maintained excellent structural stability over multiple cycles and allowed easy separation. Furthermore, the catalyst exhibited over 90% efficiency in the reduction of other common nitroaromatic pollutants, underscoring its versatility and applicability in wastewater treatment. This work provides a sustainable and practical solution for wastewater treatment by transforming hazardous contaminants into valuable aromatic amines using an easily separable catalytic system.
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RARE METALS
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2026
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IF 11
Fan Xue,Liang Chen,Xindong Zhu,Jianrong Zeng,He Zhu,Si Lan
en This link goes to a English section zh This link goes to a Chinese section Precise control of chemical ordering in bimetallic nanocatalysts offers a route to decouple activity and selectivity in acetylene hydrogenation, but direct atomic-scale evidence linking surface order to catalytic performance is scarce. Here, we tune Pd-Cu nanoalloys from chemically disordered to highly ordered states by composition control and targeted H 2 thermal treatment. Under near-industrial conditions, all catalysts reach full acetylene conversion between 100°C and 120°C, whereas the ethylene selectivity enhances with the chemical ordering increasing. By combining synchrotron X-ray absorption fine structure (XAFS) with X-ray total scattering and reverse Monte Carlo (RMC) simulation, three-dimensional atomic models are reconstructed to quantitatively map surface coordination. Compared with the chemically disordered Pd-Cu nanocatalyst, the highly ordered PdCu shows an increase in average surface Pd-Cu coordination and an expansion of mean surface Pd-Pd separations. These structural features weaken ethylene binding and suppress re-adsorption, rationalizing the enhanced selectivity. Our study provides direct atomic-scale evidence connecting chemical order to catalytic selectivity and opens the way for guiding the precise design of bimetal nanocatalysts. 摘要 en This link goes to a English section zh This link goes to a Chinese section 精准调控双金属纳米催化剂的化学有序,可为乙炔加氢反应中活性与选择性的解耦提供有效路径。然而将表面有序度与催化性能直接关联的原子尺度证据仍较为缺乏。本研究通过成分调控与氢气热处理,成功实现了Pd-Cu纳米合金从化学无序态到高度有序态的转变。在近工业条件下,所有催化剂均在100–120°C区间内实现乙炔完全转化,而乙烯选择性随化学有序度的提升显著增强。结合同步辐射X射线吸收精细结构谱、X射线全散射及反向蒙特卡洛(RMC)模拟,我们重构了纳米合金的三维原子结构模型,实现了表面配位环境的定量解析。与化学无序的Pd-Cu纳米催化剂相比,高度有序的PdCu合金表现出更高的表面Pd–Cu配位数和更长的平均Pd–Pd键距。这些结构特征有助于弱化乙烯吸附并提高其选择性。本研究为化学有序与乙烯选择性之间的关联提供了直接的原子尺度证据,为双金属纳米催化剂的精准设计开辟了新途径。
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ACS Catalysis
·
2026
·
IF 13.6
Shufen Ma,Yachao Wang,Guofeng Zhao,Weixin Huang,Cong Fu
Photocatalytic oxidative dehydrogenation of ethane (ODHE) is a promising route to ethylene under mild conditions, yet achieving a high yield and selectivity is challenging due to the inert C–H bonds and overoxidation to CO2. In this study, we present ZnO fine nanoparticles decorated with highly dispersed Pd species and featuring closely associated interfacial oxygen vacancies (Ov) for highly selective ODHE. The optimized catalyst achieves a C2H4 production rate of 8.5 mmol g–1 h–1 with a selectivity of up to 96.1%, surpassing most reported photo- and thermocatalysts and maintaining robust stability for over 10 h. Through a combination of operando DRIFTS, in situ XPS, and in situ EPR analyses, we demonstrate that the enhanced photocatalytic performance stems from a synergistic, spatially separated dual-site configuration involving Pd species and adjacent interfacial Ov. This configuration enhances spatial charge separation, promotes oxygen activation, and facilitates the selective conversion of C2H6 into key *C2H4 intermediates, thereby boosting ethylene formation. This work not only provides fundamental insights into the photocatalytic ODHE mechanism but also underscores the importance of interfacial engineering in the design of highly efficient photocatalysts for alkane conversion.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2026
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IF 9.2
Jiangtao He,Xinwei Wang,Ming Gao,Yugang Su,Hongsheng Jia
Magnesium hydride (MgH 2 ) suffers from sluggish kinetics and high operational temperatures, hindering practical hydrogen storage. We pioneer a spatially decoupled catalytic strategy that assigns distinct roles to Ti 0 . 10 Zr 0 . 15 V 0 . 35 Cr 0 . 10 Ni 0 . 30 (TA) alloy (bulk diffusion promoter) and Pd/C (surface dissociation catalyst), overcoming the inherent coupling of rate-limiting steps in MgH 2 . This design achieves near-ambient absorption (4.56 wt% at 100 °C) and eliminates activation cycles—a milestone unattained by single-catalyst systems. Kissinger analysis confirms a 46.0% reduction in activation energy (78.8 kJ/mol) for the surface-limited step, directly validating the spatial separation of catalytic functions. Crucially, the composite retains 92.3% capacity after 30 cycles with negligible kinetic degradation (0.40% decay/cycle), eliminating the need for activation. This work establishes a spatially coupled catalytic mechanism that decouples surface and bulk processes, enabling a lower operating temperature for MgH 2 .
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CHINESE JOURNAL OF CATALYSIS
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2026
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IF 17.2
Fuhao Yin,Qianyu Zhang,Mao Xu,Shupeng Wei,Yi Li,Pengzuo Chen,Yanying Zhao,Benxia Li
Achieving efficient photocatalytic CO 2 reduction using H 2 O as a hydrogen source requires the synergistic optimization of both charge and proton transfer between CO 2 reduction and H 2 O oxidation half-reactions. However, conventional studies mostly focused on enhancing these half-reactions independently, overlooking the intrinsic interdependence between them. Herein, this work develops a photothermal catalyst (denoted as Pd 1+c /3DOM-In 2 O 3 ) through engineering synergistic Pd single atoms (Pd 1 ) and Pd clusters (Pd c ) in three-dimensional ordered macroporous (3DOM) In 2 O 3 framework. The mechanistic study reveals that the coexistence of Pd single atoms and clusters not only offers synergistic active sites to promote the reaction of CO 2 and H 2 O, but also substantially improves the separation and transfer efficiencies of photogenerated electrons and holes. The Pd clusters facilitate H 2 O dissociation to ensure an adequate supply of active hydrogen species as well as synergistically enhance the adsorption and activation of CO 2 at Pd single-atom sites. Furthermore, the enhanced photoabsorption in visible and near-infrared regions, attributed to the localized surface plasmon resonance of Pd clusters, leads to a significant increase in catalyst temperature under simulated solar irradiation. The integration of photocatalysis with the photothermal effect affords an intensified driving force for the selective conversion of CO 2 and H 2 O into CO, thereby accelerating the reaction kinetics of the overall photocatalytic CO 2 reduction process. As a result, the Pd 1+c /3DOM-In 2 O 3 catalyst exhibits excellent performance for solar-driven CO 2 reduction with H 2 O vapor, achieving a remarkable CO production rate of 192.52 μmol g –1 h –1 , which is 19.8-fold and 12.2-fold higher than those of pure 3DOM-In 2 O 3 and Pd 1 /3DOM-In 2 O 3 , respectively. This study provides valuable insights into the synergistic effect of metal single atoms and clusters toward both efficient photocatalysis and photothermal effect for solar-driven CO 2 reduction.
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Journal of the American Chemical Society
·
2026
·
IF 16.6
Mimi Wu,Junzhong Xie,Guangyou Huo,Xiaolin Yu,Xueqin Yang,Yi Xing,Wei Su,Yang Zheng,Yuechang Wei,Maofa Ge,Ding Ma
Precise engineering of the metal–support interaction (MSI) is paramount for manipulating the geometric and electronic structures of supported metal catalysts, yet tailoring the local anchoring microenvironment at the atomic level remains a challenge. This study demonstrates how modulating the hydroxyl chemistry on CeO2 can direct the MSI to stabilize distinct Pd species─from single atoms to subnanometric PdOx ensembles. We show that conventional terminal hydroxyl groups on CeO2 favor the anchoring of Pd single atoms, whereas engineered bridging hydroxyl nests effectively confine undercoordinated PdOx clusters. This PdOx ensemble results in a moderate 4d orbital occupancy of Pd sites, which optimizes the σ-electron-acceptance and back-donation processes critical for C–H bond activation. Consequently, the PdOx ensemble catalyst achieves a dramatic decrease in methane combustion temperatures (T50 and T90 values are 340 and 402 °C, lowered by 175 and 226 °C, respectively) compared to the single-atom counterpart, alongside exceptional stability and water resistance under practical conditions. This work establishes the engineering of the support’s hydroxyl microenvironment as a powerful strategy for designing highly efficient metal ensemble catalysts.
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