CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Luoqi Xie,Fei Liu,Shangyan Zhou,Jiamin Wang,Jinjin Sun,Zaiyin Hu
A Pd-MX/GaZnZrO x hybrid catalyst was developed for CO 2 hydrogenation. • MXene acts as a hydrogen-delivery platform beyond a conventional support. • Interfacial coupling promotes H 2 activation and CO 2 conversion synergistically. • A methanol STY of 600.2 mg gcat −1 h −1 was achieved at 320 °C. • DFT and DRIFTS confirm an accelerated formate-mediated pathway. Efficient CO 2 hydrogenation to methanol requires a balanced interface where CO 2 activation is coupled with H 2 dissociation and subsequent hydrogenation. Herein, a Pd-modified MXene (Pd-MX)/GaZnZrO x hybrid catalyst was developed by integrating Pd-modified MXene with Ga-modified ZnZrO x oxide to overcome the limited hydrogen activation ability of Cu-free oxide catalysts. In this architecture, Pd provides H 2 dissociation sites, GaZnZrOx contributes to CO 2 adsorption and activation through its surface oxygen-related sites, and promotes the formation and hydrogenation of formate- and methoxy-related intermediates. Under 320 °C, 3.0 MPa, H 2 /CO 2 = 4:1, and GHSV = 24,000 mL gcat −1 h −1 , Pd-MX/GaZnZrO x achieved 10.5% CO 2 conversion, 83.26% methanol selectivity, and a methanol space-time yield of 600.2 mg gcat −1 h −1 , outperforming GaZnZrOₓ and Pd/GaZnZrO x while maintaining stability over 100 h. Spectroscopic characterization and DFT calculations reveal that MXene coupling enriches electrons on Pd, facilitates H 2 activation, improves interfacial adsorption behavior, and stabilizes formate- and methoxy-related intermediates. These results support a contact-dependent Pd-MX/GaZnZrO x architecture that enhances H 2 activation and facilitates the hydrogenation of CO 2 -derived intermediates over the Cu-free oxide catalyst. Download: Download high-res image (153KB) Download: Download full-size image
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Biology Direct
·
2026
·Vol. 21
·期 1
·177
·
IF 5.5
Sun Tian-qi,Wu Shuo,Qiao Jing,Liang Gang,Liu Chao-feng,Jiang Hui-yu,Liu Kai-yuan,Wang Hai-long,Pang Min
Non‑small cell lung cancer (NSCLC), particularly lung adenocarcinoma (LUAD), exhibits a high rate of primary resistance to immune checkpoint inhibitors, underscoring the need to decipher the molecular mechanisms of immune evasion. Here, we identify ANKRD49 as a critical regulator of PD‑L1 expression and immunosuppression in LUAD. Immunohistochemical analysis of clinical LUAD specimens revealed that high ANKRD49 expression correlates with reduced CD4 + and CD8 + T cell infiltration, increased FOXP3 + regulatory T cells, and elevated PD‑L1 levels. Functional experiments demonstrated that ANKRD49 overexpression in LUAD cells suppresses T cell cytotoxicity, promotes T cell apoptosis, and impairs granzyme B and IFN‑γ production in vitro. Mechanistically, ANKRD49 directly binds the transcription factor MEF2A via its second ankyrin repeat domain, upregulates MEF2A expression, and promotes its transcriptional activity at two specific sites within the PD‑L1 promoter. Chromatin immunoprecipitation and luciferase reporter assays confirmed that MEF2A directly activates PD‑L1 transcription in an ANKRD49‑dependent manner. In subcutaneous and metastatic mouse models, ANKRD49 overexpression accelerates tumor growth and metastasis, while PD‑L1 blockade reverses these effects and restores antitumor immunity. Collectively, our findings establish the ANKRD49–MEF2A–PD‑L1 axis as a novel driver of immune evasion in LUAD, and identify ANKRD49 ankyrin repeat domain 2 as a potential therapeutic target for overcoming immunotherapy resistance.
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ACS Applied Polymer Materials
·
2026
·
IF 5.2
Yiwei Li,Xu Jiang,Chuntao Chen,Xiao Fu,Dongping Sun
The dense stromal barrier of pancreatic cancer (PC) severely limits chemotherapeutic efficacy. Although combination therapy is a standard clinical approach, it often exacerbates systemic toxicity. To address the dual challenges of localized drug delivery and immune activation, we developed an injectable, multifunctional hydrogel system for the synergistic codelivery of an anti-PD-1 antibody and chemotherapeutic agents (gemcitabine/albumin-bound paclitaxel). This system is based on a novel, fully natural-source composite material─methacrylated silk fibroin (SilMA) and methacrylated chitosan (CSMA). Its core innovations include: in situ gelation via a mild LAP-photoinitiation process preserves antibody bioactivity and bioactive degradation products derived from the natural polymers, which may help establish a favorable peritumoral microenvironment. In an orthotopic PC mouse model, a single peritumoral injection of this hydrogel (HLGP group) significantly enhanced tumor infiltration of CD8+ T cells, suppressed tumor growth, and outperformed all control groups, including the free-drug combination group. This study presents a unique, integrated local delivery strategy capable of simultaneously overcoming the stromal barrier, reducing systemic exposure and enhancing immunotherapy efficacy, thereby offering a promising translational pathway for the treatment of pancreatic cancer.
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NEW JOURNAL OF CHEMISTRY
·
2026
·
IF 2.6
Xiaoxia Tian,Shuxin Liu,Jiuzhou Zhao,Jiayao He,Liang Xian
In this paper, copper-doped N-containing carbon materials (CuCN) were obtained by pyrolyzing copper acetylacetonate using a metal–organic skeleton (ZIF-8) at 900 °C. Pd/CuCN nanomaterials were synthesized using a photochemical method assisted by the ethylene glycol reduction strategy. The precise preparation of Pd/CuCN nanomaterials was realized by regulating different wavelengths of the light source and different precursor concentrations in the photochemical process to control the particle size, morphology, and crystal structure effectively. The results showed that the catalyst 10Pd/CuCN-3 prepared under green light at a wavelength of 550 nm and a precursor concentration of 10 mM had high catalytic activity. Its degradation rate constant for 4-NP was 1.77 min−1 and the conversion rate was maintained at about 90% after five cycles of reaction, which showed good durability and conversion rate. This study demonstrates that visible light can effectively control and prepare palladium nanoparticles of smaller size.
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Chinese Journal of Natural Medicines
·
2026
·Vol. 24
·期 3
·349-364
·
IF 7.5
Jiaying Wang,Yangfan Zhang,Haoqian Wu,Siqi Yu,Xiaoying Cai,Youying Zhang,Jian Chen,Zixing Chen,Xiao Zheng,Haiping Hao
Huperzine A (HupA) is a highly selective, reversible acetylcholinesterase (AChE) inhibitor that exhibits neuroprotective effects and is clinically used to manage benign memory decline. However, the specific relationship between the pharmacokinetic (PK) profile of HupA and cerebral acetylcholine (ACh) dynamics remains poorly characterized. Here, we characterize the PK-pharmacodynamic (PD) properties of HupA in rats under both physiological and pathological conditions. Following a single intramuscular injection, HupA exhibits a short half-life but rapid brain penetration, while multiple dosing significantly enhances its brain exposure. In a middle cerebral artery occlusion (MCAO) rat model, HupA demonstrates increased brain distribution. Furthermore, HupA elevates ACh concentrations across multiple brain regions, concurrently modulating several monoamine neurotransmitters. Using a minimal physiologically based pharmacokinetic-pharmacodynamic (mPBPK-PD) modeling approach, cerebral ACh dynamics were accurately predicted based on the pharmacokinetics of HupA in systemic circulation. The developed mPBPK-PD model exhibits robust predictive performance and holds potential for guiding the optimization of clinical dosing regimens and improving the therapeutic efficacy of HupA.
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PubMed
高影响因子
ACS Applied Nano Materials
·
2026
·Vol. 9
·期 30
·14188-14198
·
IF 5.8
Qiu Changkun,Zhu Liang,Li Qingrun,Wang Haozhi,An Fei,Wang Shiqiang,Fan Chao,Yang Zhe
Hydrogen
sulfide (H 2 S), a highly toxic and corrosive
gas, requires highly sensitive, selective, rapid, and stable trace-level
detection in various industrial settings. To address the limitations
of conventional metal oxide-based H 2 S sensors─such
as insufficient detection limits, poor selectivity, and inadequate
long-term stability─this study developed an H 2 S
sensor by integrating Pd-loaded In 2 O 3 nanomaterials
with microelectro-mechanical systems (MEMS) technology. A Pd–In 2 O 3 composite with a one-dimensional nanorod structure
was successfully synthesized via a hydrothermal method followed by
thermal treatment. Systematic characterization confirmed that Pd nanoparticles
are uniformly dispersed on the In 2 O 3 surface
in the metallic state. When fabricated into a MEMS-based sensor, the
composite exhibited excellent overall performance at near-ambient
temperature (25 ± 2 ° C): a detection limit as low as 50
ppb, response and recovery times of 8 and 13 s, respectively, a selectivity
ratio ≥5 (response to H 2 S compared to interfering
gases such as CO, H 2 , and CH 4 ), and less than
3% fluctuation in repeated tests. Theoretical calculations revealed
that the adsorption energy of H 2 S on Pd–In 2 O 3 (−0.787 eV) is more negative than that on pristine
In 2 O 3 (−0.679 eV), accompanied by a greater
charge transfer (0.124 |e| vs 0.086 |e| for pristine In 2 O 3 ). Mechanistic analysis indicated that Pd doping not
only modulates the band structure of In 2 O 3 via
an electronic doping effect (forming a Schottky junction) but also
acts as catalytic active sites, preferentially promoting the surface
oxidation of H 2 S. The synergistic effect of enhanced adsorption
affinity, accelerated charge transfer (verified by theoretical calculations),
and selective catalysis significantly improves the sensor’s
sensitivity, selectivity, and response speed. This work provides an
effective strategy for material design and device implementation in
developing high-performance, low-power, and easily integrable trace
H 2 S sensors.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2026
·Vol. 65
·期 31
·16619-16631
·
IF 3.9
Wu Xianjin,Wu Yipeng,Liu Zirui,Fu Jiawei,Li Wen,Cheng Yangjian,Wang Kuncan
Selective hydrogenation of nitrile butadiene rubber (NBR)
is a
key process for producing high-performance hydrogenated nitrile butadiene
rubber (HNBR). Nevertheless, the large molecular size (10 5 –10 6 g/mol) and strong steric hindrance of NBR
polymers lead to severe mass transfer limitations and significant
metal leaching via multiple interconnected mechanisms, resulting in
low catalytic activity and poor catalyst stability. To address this
challenge, a functionalized hierarchically porous carbon catalyst
with highly dispersed Pd NPs (Pd/CSA-AIR-300) was rationally constructed
from sodium alginate via acid etching and controlled oxidation. Oxygen-containing
functional groups derived from sodium alginate promote the high dispersion
of Pd NPs. Meanwhile, acid etching introduces abundant surface defect
sites, which further regulate the electronic structure of Pd. On the
other hand, the loose and interconnected pore structure of the carbon
skeleton significantly reduces the diffusion limitation of polymer
chains, improving the accessibility of active sites. Pd/CSA-AIR-300
(1 wt %) exhibited superior NBR hydrogenation performance over commercial
Pd/C (5 wt %), achieving 92.0% conversion and 100% C═C selectivity
at 60 ° C and 4 MPa H 2 . Herein, a synergistic strategy
combining defect engineering and oxygen-containing functionalization
of biomass-derived carbon is proposed, enabling efficient and sustainable
hydrogenation of high-viscosity polymers while reducing cost and offering
a practical route to enhance rubber properties.
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Carbon Neutralization
·
2025
·Vol. 4
·期 6
·e70080
·
IF 12
Jixin Shi,Peipei Zhang,Fawang Liu,Tiantian Su,Jingsan Xu,Chao Lin,Xiaopeng Li,Wei Luo
The development of advanced catalytic technologies for the combustion of low-concentration methane is crucial for minimizing unburned CH 4 emissions, consequently improving the eco-efficiency of natural gas vehicles and power plants. The integration of effective catalysts into existing systems with minimal modifications is of paramount importance. Porous ceramic composites offer a promising alternative to traditional powder catalysts due to their high surface area, excellent thermal stability, adjustable porosity, and prolonged catalytic durability. This study introduces a trace Pd–incorporated SnO 2 porous ceramic catalyst (Pd/SnO 2 ) fabricated using the spark plasma sintering (SPS) technique. The synthesis process uses a NaCl salt template to create a porous structure and graphite to improve Pd loading and dispersion on the SnO 2 surface. An optimized 10 wt.% graphite-decorated Pd/SnO 2 porous ceramic catalyst, containing a trace Pd loading of 0.17 wt.%, achieved a low T 90 of 427°C during methane reforming tests and maintained stable catalytic performance after multiple temperature cycling and over 900 min of continuous operation. Enhanced activity stems from two synergies: first, graphite-mediated uniform PdO dispersion boosting active site accessibility and second, PdO–SnO 2 interfacial charge transfer generating oxygen-deficient sites, accelerating CH 4 dissociation and stabilizing Pd 2+ against deactivation. These findings highlight the potential of this approach for use in the development of durable and efficient ceramic composite–based catalysts for environmental applications.
研究领域:
催化化学
·
环境工程
·
材料科学
·
陶瓷复合材料
·
能源技术
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高影响因子
Catalysis Science & Technology
·
2025
·Vol. 15
·期 15
·4515-4527
·
IF 4.2
Huawei Xie,Bei-Bei Zhang,Fang-Xing Xiao
Antimony sulfide (Sb2S3) has been deemed a promising semiconductor for solar energy conversion owing to its suitable energy level position. However, so far, Sb2S3-based photocatalytic systems have been poorly reported, making Sb2S3-dominated photocatalytic mechanisms elusive. Herein, an efficient electrostatic self-assembly strategy was developed to fabricate metal nanocrystal (NC)-functionalized Sb2S3 nanorod (Sb2S3 NRs-M, M = Au, Ag, Pd) heterostructures. The tartaric acid (TA) molecules grafted on the Sb2S3 NR surface served as coordination sites, which enabled the self-assembly of the metal precursor on the Sb2S3 NR surface via electrostatic and coordinate interactions. The as-prepared Sb2S3 NRs-M (M = Au, Ag, Pd) heterostructures demonstrated significantly enhanced photoactivities toward the mineralization of organic pollutants under visible light irradiation, surpassing those of the pristine Sb2S3 NR counterpart. The contributing role of metal NCs as “electron reservoirs” in boosting the charge separation was determined. Furthermore, active species participating in the photocatalytic reaction were determined, and the photocatalytic mechanism was unveiled. This study offers an efficacious strategy for the rational construction of metal NC-functionalized Sb2S3 NRs for widespread photocatalytic applications.
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高影响因子
JOURNAL OF POWER SOURCES
·
2025
·
IF 7.9
Liangbin Shao,Zhiqi Zhao,Na Xu,Yuanan Li,Haoze Li,Yuan Sheng,Shijie Zhang,Jianguo Wang
Deuterium (D 2 ) is a strategic material essential to the nuclear, fiber optic, and semiconductor industries. Proton exchange membrane (PEM) electrolysis of heavy water (D 2 O) is a robust and environmentally friendly method for D 2 production, but its energy efficiency is limited by the sluggish deuterium evolution reaction (DER). While being a promising DER catalyst, Pd still suffers from suboptimal DER kinetics due to strong adsorption of active deuterium (D∗). Herein, synergistic interactions between Pd and Mo/MoO x on carbon black are introduced to modulate the adsorption of active deuterium/hydrogen, leading to outstanding deuterium/hydrogen evolution performance. In 0.5 M D 2 SO 4 (H 2 SO 4 ), the optimal PdMo/C catalyst exhibits a record low overpotential of 19.1 mV (13.3 mV) at 10 mA cm −2 and a mass activity 10 times higher than that of commercial Pt/C. Furthermore, PdMo/C outperforms Pt/C in PEM electrolysis of D 2 O at 1.5–3.0 A cm −2 . X-ray photoelectron spectroscopy, DFT calculation, and D∗ underpotential deposition experiments show decreased electron density of Pd and reduced adsorption energy of D∗ in the presence of Mo that lead to enhanced intrinsic activity. This work offers valuable insights into the development of high-performance Pd-based electrocatalysts and demonstrates their potential in industrial production of D 2 .
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高影响因子
iScience
·
2021
·
IF 5.458
Qing Zeng,Danye Liu,Hui Liu,Penglei Cui,Chaoquan Hu,Dong Chen,Lin Xu,Xiang Wu,Jun Yang
Summary Deliberately optimizing the d-band position of an active component via electronic and lattice strain tuning is an effective way to boost its catalytic performance. We herein demonstrate this concept by constructing core-shell Au@NiPd nanoparticles with NiPd alloy shells of only three atomic layers through combining an Au catalysis with the galvanic replacement reaction. The Au core with larger electronegativity modulates the Pd electronic configuration, while the Ni atoms alloyed in the ultrathin shells neutralize the lattice stretching in Pd shells exerted by Au cores, equipping the active Pd metal with a favorable d-band position for electrochemical oxygen reduction reaction in an alkaline medium, for which core-shell Au@NiPd nanoparticles with a Ni/Pd atomic ratio of 3/7 exhibit a half-wave potential of 0.92 V, specific activity of 3.7 mA cm −2 , and mass activity of 0.65 A mg −1 at 0.9 V, much better than most of the recently reported Pd-even Pt-based electrocatalysts.
研究领域:
材料科学
·
电化学
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高影响因子
Chemistry-An Asian Journal
·
2021
·Vol. 16
·期 22
·3743-3747
·
IF 4.568
Min-Jie Chen,Gang-Gang Chang,Li-Yan Chen,Ke-Xin Huang,Chun Pu,Dan Li,Yao Yao,Jia-Xin Li,Xiao-Yu Yang,Banglin Chen
Graphical The core-shell catalyst with surface wrinkles greatly improves the selectivity of tandem catalysis. Process intensification, targeting the maximization of spatial-temporal productivity utilizing minimum energy and resources has always been the constant trends especially in chemical industry. In this regard, tandem reactions that are able to perform a multi-step reaction in a single pot by eliminating costly separation steps have been viewed as a typical paradigm. However, a spatial isolation of varied active sites with a controlled manner in a single catalyst to avoid deactivation and work synergistically is a challenging problem yet sometimes being overlooked. In this work, a spatial base-metal core-shell structured catalyst with wrinkled surface was successfully fabricated by a direct homoepitaxial growth method in an acid/water system, which exhibited increased hydrophobicity, exposure of active sites and significantly improved product selectivity towards one-pot Knoevenagel condensation-hydrogenation tandem reaction compared with the uncoated catalyst. Meanwhile, the catalytic performance was largely retained and the structural stability was maintained even after successive 8 cycles, which shows great promise for industrial applications.
研究领域:
化学工程
·
材料科学
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