ACS Nano
·
2026
·
IF 17.3
Ruofan Zhang,Xingxing Xie,Zanhong Deng,Jie Meng,Xiaohua Ji,Qi Zhang,Ruoqing Zhang,Siyuan Liu,Dandan Rong,Shimao Wang,Xiaodong Fang,Gang Meng
Abstract Selective detection of trace (weakly reducing) dimethyl sulfide (DMS) in highly humid exhaled breath using metal oxide semiconductor (MOS) sensors, with the presence of strong reducing H2S interference gas, is essential for the early diagnosis of hepatic diseases. However, it remains a big challenge in principle. Herein, a bilayer MOS sensor with a Pd–WO3 sensing film and a CuO/Al2O3 filtering overlayer was proposed. The temperature-dependent H2S catalytic oxidation experiment suggests that CuO could effectively filter H2S even under room temperature. Dispersing the CuO particles into insulative Al2O3 carrier could not only selectively remove H2S without significant consumption of DMS but also isolate the underlying Pd–WO3 sensing layer’s response signal from interference caused by that of CuO. By adding the CuO/Al2O3 1:9 filtering overlayer, the response ratio of DMS to H2S was significantly enhanced from 3.3 to 50.4, furthermore, an ultrahigh response (701.3) to 10 ppm DMS, and a low limit of detection of 10 ppb under 90% RH were achieved, which promises the future breath disease diagnosis.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Hongyu Yang,Yuelin Zhao,Sen Mu,Siqi Wang,Aiyang Tong,Dongkai Wang,Jiajia Jia,Ji Li
HA@CZ enables acid-responsive local Ca 2+ /Zn 2+ ion therapy. • Zn 2+ impairs Ca 2+ extrusion and drives sustained Ca 2+ overload. • Dual-ion stress induces caspase-1/GSDMD and caspase-3/GSDME pyroptosis. • HA@CZ cascade-induces pyroptosis and activates the STING pathway. • Local HA@CZ treatment sensitizes 4 T1 tumors to PD-1 blockade. Triple-negative breast cancer responds poorly to immune checkpoint blockade, partly because of insufficient tumor-local immune priming. Controlled delivery of bioactive ions offers an opportunity to induce inflammatory tumor cell death while limiting nonspecific systemic exposure. Here, we developed hyaluronic acid-modified, zinc containing calcium carbonate nanoparticles (HA@CZ) for acid-responsive synchronized Ca 2+ /Zn 2+ delivery. HA@CZ remained colloidally stable under physiological conditions but released Ca 2+ and Zn 2+ more rapidly under tumor relevant acidic conditions. HA@CZ markedly promoted intracellular Ca 2+ /Zn 2+ accumulation, induced mitochondrial dysfunction, and triggered gasdermin dependent pyroptosis through the caspase-1/GSDMD and caspase-3/GSDME axes. Mechanistically, the key distinction of HA@CZ does not lie in Ca 2+ overload alone, but in converting Ca 2+ overload from a direct ion burden process into a Zn 2+ initiated Ca 2+ homeostasis collapse mechanism. Zn 2+ impaired mitochondrial energy metabolism and ATP dependent Ca 2+ extrusion, thereby lowering the threshold for sustained Ca 2+ overload after synchronized ion release. The resulting dual ion stress promoted mitochondrial deoxyribonucleic acid leakage and activated cyclic GMP–AMP synthase stimulator of interferon genes signaling, thereby coupling tumor cell pyroptosis with endogenous deoxyribonucleic acid sensing activation. In syngeneic 4 T1 tumor models, HA@CZ suppressed tumor growth after both systemic and local administration, promoted dendritic cell maturation and CD8 + T-cell infiltration, and remodeled the tumor immune microenvironment toward a pro-inflammatory phenotype. Intratumoral studies confirmed its intrinsic therapeutic superiority over free CaCO₃, Zn 2+ , and their physical mixture, while combination with anti-PD-1 therapy enhanced control of both primary and distant tumors. Furthermore, tumor re-challenge experiments demonstrated that HA@CZ induced durable antitumor immune memory. These findings establish HA@CZ as a controlled-release ion nanotherapeutic that couples synchronized Ca 2+ and Zn 2+ delivery to pyroptosis associated immune activation and checkpoint blockade sensitization. Download: Download high-res image (150KB) Download: Download full-size image
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高影响因子
ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Yang Tang,Qun Jiang,Rongli Chen,Siqi Wu,Yichang Luo,Xi Huang,Guofang Yu,Cui Shao
Recent advances in immune checkpoint inhibitors (ICIs), particularly those targeting PD-1/PD-L1, have transformed cancer treatment. However, their efficacy is often hampered by the immunosuppressive tumor microenvironment (TME). Here, we developed a cantharidin-loaded nanomedicine (CA@TPGS-AmP), composed of D-α-tocopheryl polyethylene glycol succinate (TPGS) and naturally derived amphiphilic peptides (AmP), designed to enhance PD-1 blockade via induction of immunogenic cell death (ICD). In vitro, CA@TPGS-AmP markedly improved the solubility of cantharidin and exhibited superior penetration in 3D tumor spheroids. It effectively triggered key ICD events, including calreticulin (CRT) surface exposure, ATP release, and HMGB1 translocation, thereby promoting dendritic cell (DC) maturation. In vivo, CA@TPGS-AmP significantly augmented the antitumor efficacy of PD-1 therapy in 4T1 orthotopic breast cancer and LLC lung cancer models. Mechanistically, the combination therapy remodeled the TME into an immunostimulatory state by increasing CD8+ T cell infiltration and activation, leading to enhanced tumor suppression compared to monotherapies. These findings support CA@TPGS-AmP as a promising adjunct to PD-1 blockade and highlight the potential of natural product-based nanomedicine in advancing cancer immunotherapy.
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DOI
PubMed
高影响因子
CATALYSIS LETTERS
·
2024
·
IF 2.3
Li Jia-Kai,Li Xiang-Yu,Xu Zhong-Ning,Sun Jing,Lin Shu-Juan,Qin Qiu-Pei,Liu Bin-Wen,Wang Ming-Sheng,Guo Guo-Cong
Reduction of nitric acid reaction (2NO + HNO 3 + 3CH 3 OH → 3CH 3 ONO + 2H 2 O) can convert by-product nitric acid into raw material methyl nitrite in the coal to ethylene glycol (CTEG) technology. This not only realizes the efficient recycling of nitrogen resources but also plays a crucial role in mitigating environmental pollution. Despite being a promising catalyst, the Pd/C catalyst face challenges due to its high metal loading, substantial loss rate, and consequent issues of poor stability, presenting obstacles in meeting industrial requirements. To address this issue, a defect strategy has been employed to develop a low-loaded 0.3% Pd/NC catalyst with robust metal-support interaction, resulting in a significant enhancement of catalyst stability. Remarkably, even after undergoing five cycles, the catalyst maintains a high nitric acid conversion rate of 90%. This improved performance can be attributed to the strong metal-support interaction driven by electron transfer from the nitrogen-doped carbon (NC) substrate to the Pd nanoparticles evident in the Transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), and inductively coupled plasma (ICP) results. This interaction effectively suppresses the leaching of the active Pd nanoparticles, leading to significantly enhanced stability and a noticeable reduction in the loss rate. Raman spectrum and electron paramagnetic resonance (EPR) results can further reveal that the increase in the defect density lead to the strong metal-support interaction after nitrogen doping (pyridinic-N-dominated). These findings highlight the significant potential of the Pd/NC catalyst and its applicability in expediting the industrialization process of catalyst. Graphical Abstract
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高影响因子
Molecular Catalysis
·
2024
·
IF 3.9
Yu Chen,Ming-Yu Qi,Zi-Rong Tang
Integrating selective organic transformation and hydrogen (H 2 ) evolution in one photoredox reaction system is one of the most sustainable and promising approaches to efficiently produce solar fuels and chemicals by simultaneously utilizing photogenerated electrons and holes. Herein, through the cation-exchange engineering method, the nanoleaf-like Pd/CdS composites are gingerly fabricated for visible-light-driven receptor-free dehydrogenation of 1,2,3,4-tetrahydroisoquinoline (THIQ) to 3,4-dihydroisoquinoline (DHIQ) and H 2 under ambient conditions. The optimized electronic structure endows Pd/CdS with a narrow band gap and suitable energy band positions, thus facilitating the light harvesting as well as the separation and transfer of photoexcited charge carriers. Consequently, the Pd/CdS exhibits significantly improved photoredox activity compared to bare CdS . In-situ Fourier-transform infrared spectroscopy and electron paramagnetic resonance spectroscopy track the progression of reaction intermediates during such a dual-functional photoredox-catalyzed system, revealing that the carbon-centered radical is the key reaction intermediate in this reaction process. It is anticipated that this work would guide the rational utilization of CdS-based materials to enable simultaneous photochemical coupling of organic transformation and H 2 evolution.
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高影响因子
CATALYSIS LETTERS
·
2010
·Vol. 139
·期 1
·56-60
·
IF 2.021
Zhang Junli,Chen Xiaorong,Hu Tongjie,Zhang Yuan,Xu Kunling,Yu Yanpeng,Huang Jun
Abstract A highly improved Pd-catalyzed cyanation of aryl chlorides to corresponding benzonitriles was demonstrated in aqueous media. Moreover, Pd-catalyzed cyanation of aryl tosylates and benzenesulfonates with K 4 [Fe(CN) 6 ] was developed under the similar conditions, which extended application scope of the cyanation. Graphical Abstract
研究领域:
有机化学
·
绿色化学
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2022
·
IF 5.876
Yiquan Xie,Xiangju Meng,Shan Gao,Zhongbiao Wu,Feng-Shou Xiao
Catalytic combustion of CH 4 to CO 2 and H 2 O was studied over Pd nanoparticles supported on different siliceous zeolites ( MFI , BEA and CHA ) with γ-Al 2 O 3 as the reference support, and it was found that as supports, zeolites exert remarkable influence on the catalytic performance of methane oxidation , with the Pd catalyst (1 wt% loading) supported by siliceous MFI (ZSM-5-Si) presenting the highest activity. Over the exceptional catalyst, a complete conversion of methane can be achieved at around 380 °C, which is about 120 °C lower than the temperature needed for the Pd nanoparticles supported on γ-Al 2 O 3 (Pd/γ-Al 2 O 3 ), one of the best catalysts for the methane combustion. Physicochemical characterizations including X-ray diffraction (XRD), high resolution transmission electron microscopy (HRTEM), temperature programmed desorption of methane (CH 4 -TPD) and temperature programmed reduction of methane (CH 4 -TPR) techniques were used to acquire an idea what is behind the discrepancy in the catalytic performances of methane combustion over these Pd-based catalysts. Based on these results, it is proposed that the different methane adsorption and the oxygen migration capability are mainly related to the difference in the catalytic performances of methane combustion over these catalysts. Among these factors, the difference in the methane adsorption is critical for the different catalytic performances, as evidenced by the kinetic measurements.
研究领域:
催化化学
·
材料科学
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高影响因子
Molecular Catalysis
·
2021
·
IF 5.062
Shuhua Yang,Gaofeng Chen,Qian Guan,Haiyan Xu,Zhiwei Wang,Bing Liu,Shuliang Yang,Tingzhou Lei,Xianhai Zeng,Lu Lin
Bio-oil is a kind of viable renewable and environmentally sustainable energy, which is obtained from fast pyrolysis of biomass. However, bio-oil is not suitable for direct application due to the high content of oxygen and moisture. The upgrading of bio-oil, especially hydrodeoxygenation of bio-oil is highly demanded but remains a challenge owing to the absence of efficient and stable catalysts. Herein, an amphiphilic Pd/carbon-silica-alumina catalyst could catalytic reactions at the oil/water interface and simultaneously stabilized the oil/water emulsions, which would be highly advantageous in bio-oil upgrading. Significantly, the hydrophilicity and hydrophobicity of the catalyst could be adjusted by changing the input amount of precursor with resols, tetraethyl orthosilicate and aluminum chloride hexahydrate. In the catalytic reaction, phenol was used as a model bio-oil compound, where decalin and water were used to simulate an oil/water mixed bio-oil system. The as prepared amphipathic Pd/MCSA-24 catalyst showed the highest conversion of phenol (98.0%) and highest selectivity for cyclohexane (87.7%) at 200 °C, which presented great potential in further bio-oil upgrading applications.
研究领域:
能源化学
·
催化化学
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高影响因子
Chemistry-An Asian Journal
·
2017
·Vol. 12
·期 23
·3039-3045
·
IF 4.083
Yan Sun,Tao Wang,Ang Li,Ling Zhang,Qisheng Huo,Zhen-An Qiao
Graphical A simple and straightforward route is reported to knit benzene heterocycles to synthesize a series of hierarchical porous polymers with high surface area and abundant N sites. The N-doped porous polymers can effectively stabilize ultra-small Pd nanoparticles for solvent-free catalysis. Hierarchical porous polymers with more than one pore size distributions can effectively support noble metal catalysts and circumvent the limitation of the diffusion of the reactants, and thus exhibit both excellent catalytic activity and superior diffusive properties. Herein, we report a simple one-step Friedel–Crafts reaction to knit a series of benzene heterocycle monomers, such as indane, indoline, indole and tetrahydronaphthalene to obtain hierarchical porous polymers with high surface areas and/or abundant N sites. These polymers can be directly used to immobilize Pd ions, and stabilize Pd nanoparticles during the thermal reduction process to obtain Pd/polymer catalysts. In particular, indoline- and indole-based polymers with high N content up to 7 wt % exhibit outstanding ability to stabilize uniform ultrasmall Pd nanoparticles. The obtained Pd-polymers exhibit excellent catalytic activity in the solvent-free oxidation of benzyl alcohol with O 2 .
研究领域:
材料科学
·
催化化学
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高影响因子
Journal of Energy Chemistry
·
2026
·
IF 15.6
Mudong Tu,Wenhan Dai,JunFeng Huang,Zhe Zhao,Yantao Wang,Yahan Fang,Lanjuan Yao,Hua Li,Baodui Wang
The efficient utilization of active hydrogen (*H) in electrocatalytic processes remains a critical challenge for achieving high selectivity in nitrate reduction to ammonia (NO 3 − RR), as excessive *H often promotes the competing hydrogen evolution reaction (HER), leading to reduced Faradaic efficiency and ammonia yield. Herein, we address this issue by designing a single-atom Pd-doped Cu/Cu 2 O electrocatalyst (SA Pd–Cu/Cu 2 O) that precisely modulates *H generation and consumption. The SA Pd–Cu/Cu 2 O catalyst achieves an exceptional NH 3 yield rate of 1634.14 μg h −1 mg −1 , a NO 3 − –N conversion of 97.56%, a NH 3 –N selectivity of 98.13%, and a Faradaic efficiency of 92.13% at −0.8 V vs. RHE. In situ spectroscopic studies and density functional theory (DFT) calculations reveal that single-atom Pd sites serve as hydrogenation centers that generate moderate *H, which is efficiently consumed by nitrogen-containing intermediates, thereby suppressing HER. In contrast, nanoparticle Pd doping produces excess *H, favoring HER. This work demonstrates an innovative strategy for balancing *H utilization via atomic-scale metal doping, offering new insights into the design of high-selectivity electrocatalysts for sustainable ammonia synthesis and environmental nitrate remediation.
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高影响因子
NEW JOURNAL OF CHEMISTRY
·
2026
·
IF 2.6
Qian Wang,Rubo Fang,Heng Yuan,Xinyi Zhang,Guilong Hu,Qunfeng Zhang
To address the high consumption and cost of noble metal catalysts during the production of hexanitrohexaazaisowurtzitane (HNIW, CL-20), nitrogen-doped titanium dioxide (TN) was synthesized using urea as a nitrogen source. PdO/TN catalysts were then fabricated via a deposition–precipitation route and applied to the continuous hydrogenolysis debenzylation of hexabenzylhexaazaisowurtzitane (HBIW). Characterization by XRD, TEM, Raman, XPS, and H₂-TPR revealed that nitrogen incorporation effectively promoted the generation of surface oxygen vacancies and strengthened metal–support interactions, thereby enhancing catalyst stability. Moreover, the oxygen vacancy concentration could be tuned by adjusting calcination conditions. The PdO/TN-400-2 catalyst, prepared at 400 °C for 2 h, exhibited the highest catalytic activity, with an oxygen vacancy fraction of 19.64%. Further decreasing the calcination severity increased defect density but did not yield additional performance gains. These findings demonstrate that nitrogen doping can regulate surface defect chemistry and metal–support coupling, offering a viable strategy for the design of efficient catalysts for hexabenzylhexaazaisowurtzitane (HBIW) debenzylation.
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高影响因子
JOURNAL OF ORGANIC CHEMISTRY
·
2024
·
IF 3.3
Zhikang Chen,Jiahao Liu,Weiying Ou,Terumasa Kato,Zhe Wang,Yong Chen,Yan Liu,Keiji Maruoka
A series of novel axially chiral pyridylidene amine (PYE) ligands has been developed, and their catalytic capability has been demonstrated in various highly efficient and enantioselective Pd-catalyzed asymmetric allylic substitutions. A density-functional theory (DFT) study explains the preferential enantiocontrol in the key transition states of the axially chiral PYE ligand-promoted Pd-catalyzed allylic alkylation.
研究领域:
有机化学
·
催化化学
·
理论化学
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PubMed
高影响因子
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