Journal of the Taiwan Institute of Chemical Engineers
·
2020
·
IF 4.794
Guochen Zhang,Jianjun Chen,Yang Wu,Xi Liu,Pengfei Qu,Puqing Shen,Lin Zhong,Yaoqiang Chen
Natural gas vehicles (NGVs) have less CO 2 emission and have been attracting more attention. However, catalyst is needed to remove pollutants such as CO, NO x and unburned methane in NGVs’ exhausts. The development of catalysts with high resistance to chemical poisoning, especially to phosphorus poisoning induced by lubricating oil of NGVs’ engine, is a challenge. Herein, we developed a new strategy to improve the phosphorus resistance of model palladium catalyst using phosphate-modified alumina as support for NGVs. The catalysts were analyzed by N 2 -physisorption, X-ray fluorescence spectrum (XRF), X-ray diffraction (XRD), CO-chemisorption, in-situ DRIFTS and X-ray photoelectron spectrum (XPS). The results show that phosphate-alumina support helps the model catalyst maintain its textual properties, otherwise phosphorus species from lubricating oil would deposit on the surface of catalyst and block the catalytically active sites. Moreover, the relative content of active Pd 0 on phosphate-modified alumina support will not decrease. Therefore, compared with conventional Pd catalyst on alumina, the model Pd catalyst on phosphate-modified alumina can show significantly enhanced phosphorus resistance under operating conditions for NGVs, and can nearly maintain its catalytic performance of removing pollutants upon phosphorus poisoning. Our work would provide a general method for development of catalyst with high performance for NGVs.
✓ 已验证
DOI
高影响因子
Materials Today Bio
·
2026
·
IF 11
Chen Chen,Jiancong Xie,Yunsheng Zheng,Guanxiu Chen,Tingting Yin,Jie Cao,Ziyang Cao
Chemotherapy frequently induces compensatory PD-L1 upregulation in tumor cells. This adaptive response limits the durability of immune checkpoint blockade and contributes to therapeutic resistance. To overcome this barrier, we engineered an injectable hydrogel system (G-DMNP/Met) for sustained, localized PD-L1 degradation. The hydrogel continuously releases PEGylated doxorubicin-Mn 2+ chelate nanoparticles (DMNP) and metformin (Met) within the tumor microenvironment. This design enforces persistent depletion of PD-L1 and sensitizes tumors to chemo-immunotherapy. Unlike antibody-based PD-1/PD-L1 blockade, which transiently interrupts receptor-ligand engagement, our strategy directly reduces total PD-L1 protein levels. Continuous degradation prevents chemotherapy-induced PD-L1 rebound and reverses compensatory immune tolerance at its source. Local released DMNP induces immunogenic cell death and activates the cGAS-STING pathway via Mn 2+ -mediated signaling. This process enhances interferon-gamma (IFN-γ) production and restores cytotoxic T lymphocyte priming and effector function. Concurrently, sustained Met release further accelerates PD-L1 degradation, alleviates post-chemotherapy immunosuppression, and promotes effector T-cell infiltration. In vivo, this triple-synergistic approach, PD-L1 degradation, immunogenic cell death induction, and cGAS-STING activation, robustly amplifies antitumor immunity and effectively suppresses immune-cold colorectal tumors under chemotherapeutic conditions. This work presented a protein degradation-driven chemo-immunotherapy paradigm that overcomes chemotherapy-induced adaptive immune resistance and potentiates durable therapeutic responses.
✓ 已验证
产品关联
DOI
高影响因子
Small
·
2026
·
IF 11.8
Hui Wang,Xiang Li,Zitong Jiang,Qing Xu,Qiaoqin Guo,Chaozheng He,Junjun Zhang,Yaming Liu,Mingshang Jin
Direct ethanol fuel cells are promising clean energy devices, but the difficulty in cleaving the C─C bond of ethanol leads to low C1 pathway selectivity (typically ∼10%) and incomplete energy conversion. To address this challenge, we synthesized a porous multiphase Pd-based metallene nanocatalyst co-doped with oxygen-philic Cu and W. Temperature was identified as the key factor regulating the crystal structure: low temperatures yielded amorphous phases, high temperatures produced crystalline phases, and intermediate temperatures formed the desired crystalline/amorphous mixed multiphase structure. This multiphase structure provided abundant active sites. The optimal PdCuW metallene exhibited exceptional performance for ethanol electrooxidation: a record-high C1 pathway selectivity of 72.6% (1.6 times that of undoped Pd metallene and 10.2 times that of commercial Pd/C), a mass activity of 4301.6 mA/mg Pd (4.7 times that of commercial Pd/C), and superior stability (only 7.3% activity decay vs. 67.9% for commercial Pd/C). Mechanistic studies (In situ ATR-FTIR, DFT calculations) revealed that synergistic Cu-W doping reduced the C─C bond cleavage energy barrier, enhanced OH * adsorption, and weakened the poisoning effect of intermediate CO * . The work offers a rational design strategy for high-selectivity electrocatalysts, advancing ethanol's full energy utilization and holding broad implications for Pd-based catalyst systems in energy conversion technologies.
✓ 已验证
DOI
PubMed
高影响因子
Materials Today Chemistry
·
2026
·
IF 7.4
Lin Zhang,Hai-Yan Guo,You-Qiang Yao,Lu Zhang
Pyrazine-modulated PdCu electronic structure enables selective EGOR and HER • Bimetallic synergy and N-coordination boost EG adsorption and *OH generation. • The assembled-cell achieves > 97.77% GA selectivity at ultra-low voltage. • The system requires only 2.89 kWh per m 3 for H 2 , coupled with GA upgrading. Electrocatalytic ethylene glycol oxidation (EGOR) represents a promising route for co-producing value-added chemicals and hydrogen, yet achieving high selectivity and efficiency remains challenging. Herein, we report a bifunctional N-PdCu@Ni(OH) 2 nanosheet catalyst that exhibits exceptional performance for both EGOR and the hydrogen evolution reaction (HER). The material features pyrazine-N-coordinated Pd–Cu dual-sites, where Pd serves as the main active center for EG and *OH adsorption, while Cu doping electronically modulates Pd to enhance glycolic acid (GA) selectivity and promote *H adsorption for improved HER kinetics. In a membrane-free flow cell, the catalyst enables current densities of 100 mA cm −2 at only 1.20 V, with GA selectivity exceeding 97.77% and hydrogen Faradaic efficiency near 100%. The system requires only 2.89 kWh per m 3 H 2 produced, demonstrating a viable strategy for electronic modulation in multifunctional electrocatalysis and advancing low-energy hydrogen production coupled with sustainable biomass upgrading. Download: Download high-res image (525KB) Download: Download full-size image
✓ 已验证
产品关联
DOI
高影响因子
BIOMATERIALS
·
2026
·
IF 13.6
Shengjie Sun,Yixuan Fang,Huisong Hao,Jiayin Yu,Yang Zhou,Simin Wen,You Li,Tianqi Wang,Mian Yu,Meiying Wu
As the most prevalent subtype of colorectal cancer, microsatellite-stable colorectal cancer (MSS CRC) is resistant to T cell-focused immune checkpoint blockade due to its low mutational burden and immunosuppressive tumor microenvironment. Despite reprogramming tumor-associated macrophages toward a tumoricidal M1-like state being a promising alternative, its efficacy is limited by paradoxical upregulation of programmed cell death-ligand 1 (PD-L1) on M1-like macrophages and their inherently poor antigen cross-presentation capacity. Here, we report that poly-metformin (PMet) can mimic the intracellular domain of PD-L1, competitively inhibit the membrane anchoring of PD-L1, and thereby effectively downregulate cell-surface PD-L1. To evaluate the therapeutic efficacy of PMet in immunosuppressive MSS CRC, we further developed an oral probiotic outer membrane vesicle gene delivery system, si Ythdf2 /PMet@Akk-OMV, and demonstrated its ability to reduce PD-L1 levels on both macrophages and tumor cells while synergistically enhancing macrophage cross-presentation of tumor antigens, leading to potent activation of specific antitumor immunity and significant tumor growth inhibition. This work thus provides both theoretical and experimental foundations for treating cancers resistant to traditional immune checkpoint blockade therapy.
✓ 已验证
产品关联
DOI
高影响因子
ChemistrySelect
·
2026
·Vol. 11
·期 30
·e74077
·
IF 2.3
Ke Zhang,Fei Liu,Tingting Cao,Min Deng,Mengqin Yao,Xiaodan Wang
Designing catalysts with high activity and excellent stability is crucial for hydrogen production via formic acid decomposition. Considering the support properties considerably affect Pd dispersion, we designed Pd-based catalysts using Roxburgh pear residue activated by KOH, H 3 PO 4 , and ZnCl 2 . Among them, KOH activation delivered the best performance, with Pd/Cr–KOH exhibiting a turnover frequency of 963 h −1 at 303 K. This superior activity arises from the synergistic effects of the KOH-activated support. Specifically, the high specific surface area and abundant mesopores ensure uniform Pd dispersion and expose more active sites. The retained alkaline sites promote formic acid deprotonation and accelerate C–H bond cleavage. Meanwhile, oxygen-containing functional groups anchor Pd precursors, prevent metal agglomeration, and enhance electron transfer from Pd to the support, which weakens the Pd–H bond strength and facilitates H 2 desorption. These results demonstrate that KOH-activated biochar is a promising support for efficient hydrogen production from formic acid. Graphical This study designs Pd-based catalysts using KOH-, H 3 PO 4 -, and ZnCl 2 -activated Roxburgh pear residue. Pd/Cr–KOH exhibits the highest activity (TOF = 963 h −1 at 303 K) due to its high surface area, abundant mesopores, retained alkaline sites, and oxygen-functional groups that enhance Pd dispersion, promote deprotonation, weaken Pd–H bonds, and facilitate H 2 desorption.
✓ 已验证
产品关联
DOI
高影响因子
ELECTROANALYSIS
·
2026
·Vol. 38
·期 7
·e70185
·
IF 2.6
Mansoor Ahmad,Neha,Dongdong Lv,Naseer Ahmad,Guixun Yang,Wei Sun
Zinc ion (Zn 2+ ) detection is critically important in both environmental and biological systems. Although Zn 2+ plays an important role in metabolic processes, excessive intake can lead to toxic effects, highlighting the need for simple and effective detection methods for Zn 2+ . In this study, palladium nanoparticle-decorated reduced graphene oxide (Pd@rGO) nanocomposite was drop-cast onto a glassy carbon electrode (GCE) to develop a facile electrochemical sensing platform, and the resulting Pd@rGO/GCE was successfully used for the sensitive and selective detection of Zn 2+ . The morphology and structural properties of the nanocomposite were systematically characterized using Fourier transform infrared spectroscopy, scanning electron microscopy, transmission electron microscopy, X-ray diffraction, and X-ray photoelectron spectroscopy. Cyclic voltammetry and electrochemical impedance spectroscopy were used to confirm improved electrochemical performances of the modified electrode. The sensor was linear with a detection range of 2.0–200.0 µM with a low limit of detection of 1.7 nM for Zn 2+ analysis using differential pulse anodic stripping voltammetry. Moreover, the practicability of the Pd@rGO/GCE was proved by the precise Zn 2+ determination in drinking water sample.
✓ 已验证
产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2026
·
IF 6.6
Gaoqing Cao,Zhimin Feng,Haitao Yuan,Shiyue Ren,Yue Lei,Lihong Hu,Yingnan Duan,Weizun Li,Zhurui Shen
Cd vacancies precisely anchor Pt/Pd sub-nanoclusters to boost interfacial electron transfer. • The vacancy-stabilized PtPd interface steers the CO 2 reduction pathway toward CH 4 . • DFT and in situ DRIFTS unveil stabilized intermediates (*CH 3 O) and suppressed CO desorption. • The optimized catalyst achieves a 119.5-fold enhancement in CH 4 yield over pristine CdS. Selective photoreduction of CO 2 to deeply hydrogenated products remains challenging due to the competitive formation of CO and insufficient surface hydrogenation capability. Herein, a vacancy-stabilized Pt/Pd sub-nanoclusters interface is constructed on a Cd-based semiconductor to preferentially facilitate surface reaction pathways toward CH 4 production. Cd vacancies are proposed to serve as preferential anchoring and electronic modulation centers, promoting the formation of Pt/Pd interfacial sites with strong metal support interactions, and facilitating electron transfer. Multiple characterization techniques confirm that the Pt/Pd sub-naoclusters interface is preferentially stabilized at vacancy-rich regions and exhibits pronounced electronic coupling. In situ DRIFTS reveals the emergence of key hydrogenated intermediates on the Pt/Pd interfacial surface, indicating a surface-mediated pathway shift from CO desorption to deep hydrogenation. Density functional theory (DFT) calculations further confirm enhanced CO 2 activation and stabilization of hydrogenation intermediates at the vacancy-coupled Pt/Pd sub-nanoclusters. Compared to pristine CdS and Cd 1-x S, the Pt/Pd-Cd 1-x S photocatalyst achieved 119.5-fold and 14.9-fold enhancements in CH 4 yield, respectively. Consequently, the engineered interfacial surface achieves a significantly enhanced methane selectivity during CO 2 photoreduction. This work highlights the important role of vacancy-mediated dual metal interfaces in promoting surface reaction pathways and provides new insights into the rational design of selective CO 2 photoreduction catalysts from a surface science perspective. Download: Download high-res image (169KB) Download: Download full-size image
✓ 已验证
DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2026
·
IF 5.4
Fu-Rui Teng,Hao Zheng,Si-Chen Tan,Li-Ling Fu,Yue Huang,Lin Zhu,Di Wu,Ai-Dong Li
The Pd NPs@MXene/PVA hydrogel strain sensor achieves an ultra-wide strain range from 10% to 1680% with high gauge factor of 18.4. • The sensor demonstrates self-healing with 98.4% efficiency in 25 s, retains 75% of tensile strength and 89% strain capacity. • Hydrogen bonding and Pd NPs enhance mechanical performance, with tensile strength of 60.8 kPa and fracture strain of 1680%. • Sensor array integrated into smart glove enables object grasping and 0–9 gesture recognition, showing potential for human–machine interfaces. Hydrogel strain sensors are promising for electronic skin due to their flexibility and biocompatibility, yet balancing mechanical robustness, sensing performance, and self-healing remains challenging. Here, we develop an optimized Pd nanoparticles (Pd NPs)-decorated MXene/polyvinyl alcohol (PVA) hydrogel strain sensor (Pd NPs@MXene/PVA) with enhanced multifunctionality. Mechanically, the hydrogel achieves a tensile strength of 60.8 kPa and fracture strain of 1680%, outperforming pristine PVA hydrogel (17.3 kPa, 800%) through dynamic borate ester, hydrogen bonding and Pd NP reinforcement. For sensing, it provides repeatable responses over 100%–1500% strain, with cyclic stability validated at 200%–600%. Detectable responses from 10% to 1680% were observed under monotonic loading, and the maximum GF reached 18.4 in the 1200%–1680% regime. The device responds rapidly (600–700 ms) and was evaluated over 5000 stretching–releasing cycles, with the response becoming markedly more repeatable after an initial conditioning stage. Notably, it achieves 98.4% electrical self-healing efficiency within 25 s, retaining 75% tensile strength and 89% strain capability after healing, which is attributed to the dynamic borate ester bonds between PVA chains and tetraborate ions, together with reversible hydrogen-bonding interactions among PVA, MXene, and Pd NPs. Integrated into a smart glove, the sensor array distinguishes object grasps, generates distinguishable resistance patterns for digit gestures 0–9 and achieves high-accuracy MLP-based classification of digits 1–9, validating its practicality for human-machine interfaces. This work advances hydrogel sensor design by integrating Pd NPs for optimized multifunctionality, offering a robust platform for next-generation electronic skin. Download: Download high-res image (152KB) Download: Download full-size image
✓ 已验证
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2026
·Vol. 65
·期 35
·18713-18724
·
IF 3.9
Li Jianding,Hu Yanling,Zhang Linfeng,Liu Tingli,Wu Jinwen,Zhou Xuan,Jiang Ning,He Liqing,Zheng Yun,Zhu Yongyang
The rational design of catalyst supports to achieve optimal
metal-support
interaction is critical for advancing Pd-based electrocatalysts for
formic acid oxidation. Herein, we reported a thermally driven strategy
to modulate the chemical state of sulfur on carbon support derived
from propanethiol-functionalized carbon, which enabled bidirectional
tuning of the Pd state and fundamentally altered the reaction pathway
of formic acid oxidation. With an optimized calcination temperature
of 700 ° C, the Pd/SC-700 catalyst, featuring an exclusive thiophenic
sulfur configuration, exhibited the strongest metal-support interaction,
delivering an exceptional mass activity of 2222 mA mg –1 (8.3 times that of Pd/C), considerably superior stability (14 times
that of Pd/C), and faster charge-transfer kinetics for formic acid
oxidation. Gas chromatography analysis revealed a marked shift in
reaction selectivity. Although CO remained the dominant product, its
fraction dropped from 95.4% on Pd/C to 73.2% on Pd/SC-700, while the
emergence of 7.2% CO 2 directly confirmed activation of
the direct dehydrogenation pathway. Kinetic analysis showed a linear j – v 0.5 relationship ( j = 0.62 + 0.204 v 0.5 ), indicating
diffusion-controlled behavior with enhanced mass transport. This work
provides a new strategy of thiol modification followed by thermal
treatment that offers a simple yet scalable route to synthesize high-performance
anode electrocatalysts for direct formic acid fuel cells.
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Nano Materials
·
2026
·
IF 5.8
Yumin Shen,Jianwei Chen,Yueyang Sun,Xinru Yao,Lei Tang,Jiali Wang,Fangfang Zhou,Hong Duan,Joseph Irudayaraj,Lingyan Zheng,Gang Chen,Baoguo Sun
Precise structural modulation of Pt-based nanozymes is an effective strategy to enhance the catalytic performance for biochemical sensing. Herein, we report three-dimensional (3D) hollow nanospheres (HNPs) featuring highly dispersed Pd/Pt atomic sites as an efficient peroxidase mimic. The Pd/Pt-HNPs exhibit markedly enhanced peroxidase-like activity, which we attribute to the synergistic catalysis of bimetallic active centers combined with the hollow 3D architecture. Kinetic analysis reveals a Vmax of 20.29 × 10–8 M·s–1, corresponding to an activity ∼10-fold higher than that of Pd-HNPs and ∼1.6-fold higher than that of Pt-HNPs. Notably, the Kcat reaches 5.44 × 105·s–1, which is approximately 103-fold greater than that of horseradish peroxidase (HRP) under the same assay conditions. Leveraging this excellent catalytic efficiency, we established an ultrasensitive colorimetric platform for H2O2 quantification (limit of detection (LOD): 1.14 μM by calculation; visual limit of detection (vLOD): 2.5 μM by naked-eye inspection), exhibiting a detection range from 2.5 μM to 12.8 mM. The Pd/Pt-HNPs-based method delivers a sensitivity 55 and 13-fold higher than those of HRP and a confirmatory method, respectively. The assay further demonstrates reliable accuracy in complex food matrices (milk, dried bean curds, and chicken feet), affording good recovery rates (91.36–115.71%) with a coefficient of variation in the range from 4.06 to 15.41% and low susceptibility to interference. This study highlights the synergistic effect of Pd/Pt bimetallic sites and nanoengineering in enhancing nanozyme catalysis, enabling sensitive and reliable detection in complex food matrices.
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Jiabao Lv,Hongman Sun,Guanying Liu,Fangzhen Wang,Xinru Qin,Shuzhuang Sun,Youhe Wang,Zifeng Yan
Mix-ZrO 2 supports have tunable monoclinic and tetragonal crystalline phases. • InPd/Mix-ZrO 2 –400 achieves 11.5% CO 2 conversion and 52% methanol selectivity. • The specific composition improves H 2 dissociation and CO 2 adsorption. • Methanol synthesis over InPd/Mix-ZrO 2 proceeds via the formate pathway. Upgrading CO 2 to methanol represents a pivotal strategy for achieving carbon neutrality, yet the development of highly efficient indium-based catalysts remains constrained by the urgent need for precise modulation of the support structure. Herein, we rationally design an In Pd catalyst supported on mixed crystal phase ZrO 2 (Mix-ZrO 2 ) with tunable monoclinic and tetragonal fractions. The optimized InPd/Mix-ZrO 2 –400 catalyst exhibits a CO 2 conversion of 11.5% and methanol selectivity of 52% at 270 °C, significantly outperforming other comparative catalysts, and retains stability over 50 h. Crucially, the enhanced performance is intrinsically attributed to the synergistic effect derived from the specific monoclinic-tetragonal phase ratio, which significantly boosts the dissociation of H 2 and CO 2 adsorption capacity. In-situ DRIFTS analysis confirms the reaction proceeds via the formate (HCOO*) pathway, where the optimized support facilitates the rapid hydrogenation of intermediates. This work elucidates the synergistic effect of crystal phase engineering in oxide supports, offering a robust pathway for designing advanced CO 2 hydrogenation catalysts.
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）