ACS Nano
·
2026
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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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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
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
Nanotoxicology
·
2026
·
IF 3.6
Yanting Zhan,Yiyang Wu,Chanting Huang,Siyi Liu,Ke Ma,Li Zheng,Zainen Qin
The high expression of classically activated macrophages (M1) subtypes and the elevated levels of reactive oxygen species (ROS) are specifically observed in osteoarthritis (OA) patients. In this study, we synthesized a Pd@CeO2 nanozyme with a core-shell hetero-nanostructure that enhances enzyme activity through shell-core electron transfer. The goal of this work was to look into the potential of Pd@CeO2 nanozyme in scavenging ROS and regulating macrophages for the treatment of OA. The results demonstrated that the Pd@CeO2 nanozyme displayed multiple enzyme-like antioxidative activities, efficiently eliminating excessive intracellular ROS. This resulted in a significant decrease in the release of pro-inflammatory cytokines, consequently leading to a decline in the presence of M1-type macrophages. Furthermore, the Pd@CeO2 nanozyme showed excellent potential in promoting the shift of macrophages toward the M2 phenotype. Additionally, the factors secreted from the cell supernatant of Pd@CeO2-treated macrophages treated with Pd@CeO2 demonstrated anti-inflammatory properties in the chondrocytes located within inflamed synovial joints. These findings offer valuable insights into the advancement of effective enzyme-mimetic therapies for the treatment of OA.
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PubMed
高影响因子
ChemistrySelect
·
2026
·Vol. 11
·期 10
·e07382
·
IF 2.3
Tong Zhang,Haiyong Wang,Chenguang Wang,Chen Shen,Qiying Liu
Monohydric alcohols are important platform molecules with diverse applications in organic synthesis, pharmaceuticals, food, and polymer industries. The production of monohydric alcohols via the selective hydrogenolysis of diols holds significant scientific and practical value. However, the precise catalytic control of the cleavage of target C–C and C–O bonds remains an open challenge, which often leads to low yields of the target products. Herein, metal-acid bifunctional catalysts were employed to boost the conversion of diols and improve the production of monohydric alcohols through hydrogenolysis. By regulating key reaction intermediates, a maximum yield of 76.2% for 1-propanol and a total monohydric alcohol yield of 84.9% were achieved within a short reaction time of 1 h. Our investigations demonstrate that the composite system of 5% Pd/C and phosphotungstic acid (HPW) catalyzes the conversion of ethylene glycol (EG) and 1,2-propanediol via a metal-acid synergistic effect, which enables the selective cleavage of C–C and C–O bonds. Ethylene glycol and 1,2-propanediol were thus converted to the monohydric alcohols (ethanol, n-propanol, and isopropanol) through hydrogenolysis and dehydration-hydrogenation processes. Additionally, the reaction order and activation energy barriers for the conversion of diols over the 5% Pd/C catalyst were determined experimentally. This work establishes a preliminary method for the production of monohydric alcohols from the hydrogenolysis of small-molecule diols by 5% Pd/C and HPW catalysts. Given the commercial availability of these catalysts, the developed catalytic system exhibits promising practical application potential and may facilitate the scale-up of this reaction. Graphical A 5% Pd/C–phosphotungstic acid (HPW) composite catalyzes the conversion of ethylene glycol and 1,2-propanediol via metal–acid synergy, enabling selective C–C/C–O cleavage. Hydrogenolysis and dehydration–hydrogenation yield ethanol, n-propanol, and isopropanol. Reaction orders and activation energies were determined, linking mechanistic insights to industrial scale-up for biomass diol upgrading.
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高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
·
2026
·
IF 8.3
Ertai Na,Binrong Chen,Xudong Liang,Junda Li,Ruifu Ling,Xianbo Zhou,Jiayu Li,Guo-Dong Li
For the early warning of electrical fire, it is of great significance to selectively and timely detect 2-ethylhexanol (2-EH), which is a key gaseous product released from the overheated PVC covered on cables. However, the detection of 2-EH is always hindered due to the weak adsorption and activation ability of the sensing materials. Herein, we constructed dual sites contained Pd-In 2 O 3 sensor for the detection of trace 2-ethylhexanol at ppb level. In this structure, hydroxyl oxygen in 2-EH forms significant bond with In atoms, while alkyl hydrogen generates strong interaction with Pd cluster. As a result, the 0.3 Pd-In 2 O 3 sensor exhibits high response (S = 42 at 11 ppm), low detection limit (0.11 ppm) and short response time (2 s). Band structure analysis reveals that the formation of Schottky junction and spontaneous electron transfer between In 2 O 3 and Pd, leading to the improved gas-sensing performance. This work not only offers new insights into the sensing mechanism by DFT calculations but also paves the way for designing high-performance gas-sensitive materials targeted at complex organic molecules.
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高影响因子
Small
·
2026
·
IF 11.8
Hui Wang,Yanan Li,Jingjing Dou,Qing Xu,Zitong Jiang,Tao Zhang,Chaozheng He,Mingshang Jin,Xiang Li
Direct ethanol fuel cells (DEFCs) are promising clean energy devices, but their efficiency is limited by the low C-C bond cleavage efficiency of Pd-based catalysts. Herein, we synthesized In-Mo codoped Pd metallene with rich interface defects via a simple wet-chemical method, which consists of face-centered cubic, intermetallic and amorphous phases. The catalyst's structure and ethanol electrooxidation reaction (EOR) performance was systematically characterized, and the mechanism was revealed by in situ ATR-FTIR, HPLC and DFT calculations. Results showed that the optimal PdInMo metallene exhibited a C1 pathway selectivity of 73.68%, which was 12.02 time that of commercial Pd/C. Its mass activity and specific activity were 4273.8 mA mg Pd −1 and 8.36 mA cm −2 , 2.38 and 1.34 times higher than those of undoped Pd metallene (1795.9 mA mg Pd −1 and 6.25 mA cm −2 ), 6.85 and 3.83 times higher than those of commercial Pd/C (624.2 mA mg Pd −1 and 2.18 mA cm −2 ), respectively, with excellent cycling stability (75.10% activity retention). The enhanced performance was attributed to the synergistic effect of In─Mo codoping and rich interface defects: strengthened OH* adsorption, weakened CO* adsorption, and reduced C─C bond cleavage energy barrier. This study provides a novel strategy for designing high-selectivity and high-activity Pd-based catalysts for EOR.
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PubMed
高影响因子
SENSORS
·
2018
·Vol. 18
·期 5
·1448
·
IF 2.475
Han Song,Zhijie Luo,Mingyao Liu,Gang Zhang,Wang Peng,Boyi Wang,Yong Zhu
In the present work, centrifugal deposited Au-Pd core-shell nanoparticle (NP) film was proposed for the room-temperature optical detection of hydrogen gas. The size dimension of 44, 48, 54, and 62 nm Au-Pd core-shell nanocubes with 40 nm Au core were synthesized following a solution-based seed-mediated growth method. Compared to a pure Pd NP, this core-shell structure with an inert Au core could decrease the H diffusion length in the Pd shell. Through a modified centrifugal deposition process, continues film samples with different core-shell NPs were deposited on 10 mm diameter quartz substrates. Under various hydrogen concentration conditions, the optical response properties of these samples were characterized by an intensity-based optical fiber bundle sensor. Experimental results show that the continues film that was composed of 62 nm Au-Pd core-shell NPs has achieved a stable and repeatable reflectance response with low zero drift in the range of 4 to 0.1% hydrogen after a stress relaxation mechanism at first few loading/unloading cycles. Because of the short H diffusion length due to the thinner Pd shell, the film sample composed of 44 nm Au-Pd NPs has achieved a dramatically decreased response/recovery time to 4 s/30 s. The experiments present the promising prospect of this simple method to fabricate optical hydrogen sensors with controllable high sensitivity and response rate at low cost.
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高影响因子
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