Nanoscale
·
2026
·
IF 5.2
Bolong Qi,Rui Li,Haoran Jiang,Sheng Ye,Woon Yong Sohn,Zhenhua Pan
ZnIn2S4 (ZIS) is a promising visible-light photocatalyst, yet its activity and stability are severely limited by rapid charge recombination and photocorrosion. Here we report a UiO-67-mediated solid-state Z-scheme strategy to simultaneously enhance the efficiency and durability of ZIS for photocatalytic hydrogen evolution. By integrating UiO-67 with ZIS and Pt nanoparticles, an intimate heterointerface with pronounced interfacial charge redistribution is established, featuring spontaneous electron transfer from UiO-67 to ZIS. As a result, the UiO-67/ZIS/Pt composite delivers a hydrogen evolution rate 15.69 times higher than pristine ZIS, together with an apparent quantum yield of 5.94% at 380 nm and excellent cycling stability. Mechanistic studies reveal that UiO-67 functions as an interfacial charge-regulation platform that promotes Z-scheme electron flow while suppressing charge recombination. This work provides a rational approach for overcoming the intrinsic limitations of metal sulfide photocatalysts via MOF-mediated Z-scheme engineering.
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ACS Applied Materials & Interfaces
·
2026
·
IF 7.8
Tianqi Dai,Su Zhao,Yufei Qiu,Fei He,Tao Jia,Shuming Li,Jiangai Piao,Yanli Wang,Yanping Zhao,Xutong Wu,Hai Xu,Xiaoyu Zheng
Postoperative immunosuppression, which is closely associated with the oxidative-stress-driven expansion of regulatory T cells (Tregs), increases susceptibility to severe postoperative outcomes, including infectious complications, multiple organ dysfunction syndrome (MODS), and tumor progression. Here, we report a zirconium-based metal–organic framework (MOF) cascade nanozyme, designated “Pt@PCN-224-Fe”, coated with poly(ethylene glycol) (Pt@FeMOF–PEG) that simultaneously mimics superoxide dismutase (SOD) and catalase (CAT) to neutralize excessive reactive oxygen species (ROS). Mechanistically, scavenging ROS reactivates the PI3K–AKT–mTOR signaling axis, suppresses Foxp3 expression, and thereby inhibits both the differentiation of naı̈ve CD4+ T cells into Tregs under Treg-polarizing conditions and their TGF-β1 secretion in vitro. In a murine model of surgical trauma, the single intraperitoneal administration of Pt@FeMOF–PEG reversed immunosuppression within 72 h, evident as a reduced frequency of Tregs, expanded Th17 cells, normalized CD4+/CD8+ ratio, and suppressed M2 macrophage polarization (all p < 0.05). Concurrently, proinflammatory cytokines (IL-1β, IL-6, TNF-α, IFN-γ) increased, whereas anti-inflammatory cytokines (IL-4, IL-10) decreased, indicating the systemic reinvigoration of the innate and adaptive immunity. The nanozyme showed excellent biocompatibility, with negligible hemolysis (<5%), no histological organ damage, and minimal systemic toxicity. In this work, we have developed a dual-enzyme-mimicking nanozyme (Pt@FeMOF–PEG) that precisely targets the ROS–PI3K–Treg axis in a single-dose strategy to reverse postoperative immune dysfunction, thus addressing a long-unmet clinical requirement for surgical recovery.
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APPLIED CATALYSIS A-GENERAL
·
2026
·
IF 4.8
Jingyi Chen,Shuangfeng Ren,Luyao Guo,Tongtong Feng,Xiaoling Mou,Jiaxu Liu,Li Yan,Ronghe Lin,Yunjie Ding
Hydrothermal defect healing selectively stabilizes catalytically active Pt ensembles by removing weakly anchored species in Silicalite-1. • Confined Pt ensembles exhibit enhanced intrinsic activity, lower activation energy, and improved oxygen activation in aerobic alcohol oxidation. • Catalysis occurs on externally accessible Pt sites and mesoporous regions, enabling efficient oxidation of bulky alcohol molecules. • Defect-healing-induced restructuring provides a general strategy to optimize active site stability and catalytic efficiency in heterogeneous oxidation catalysts. The development of robust Pt catalysts that simultaneously achieve efficient O 2 activation, high intrinsic activity, and structural stability remains a central challenge in aerobic alcohol oxidation. Herein, we report a hydrothermal defect-healing strategy to restructure impregnated weakly anchored Pt species in Silicalite-1 zeolite into highly stable Pt ensembles confined within the zeolite framework (Pt@S-1). Spectroscopic and microscopic analyses reveal that hydrothermal treatment heals silanol defects and drives controlled restructuring of isolated Pt atoms into small ensembles strongly stabilized by the zeolitic microenvironment. The resulting Pt@S-1 catalyst exhibits markedly enhanced intrinsic activity, achieving a turnover frequency of 5560 h −1 in aqueous aerobic oxidation of 3,5,5-trimethylhexanol, exceeding conventional nanoparticle and impregnated analogues by over one order of magnitude despite significantly lower Pt loading. Kinetic studies demonstrate a reduced apparent activation energy (65.7 kJ mol −1 ) and nearly first-order dependence on O 2 pressure, indicating facilitated O 2 activation and optimized competitive adsorption between oxygen and alcohol substrates. The zeolite confinement and aqueous reaction medium synergistically promote selective formation of isononanoic acid and ester while suppressing catalyst sintering and thermal runaway. Furthermore, the catalyst shows excellent stability without requiring hydrogen pretreatment or additional base. This work establishes defect-healing-induced restructuring as an effective approach to generate stable and highly active catalytic ensembles from labile atomically dispersed precursors and provides fundamental insights into structure–activity relationships governing selective aerobic alcohol oxidation. Download: Download high-res image (150KB) Download: Download full-size image A hydrophilic zeolite-supported Pt catalyst cooperates with water to drive base-free and H 2 -free aerobic oxidation of long-chain alcohols under mild aqueous conditions, achieving selective acid formation while suppressing energy demand, metal sintering, and organic solvent use.
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ACS Omega
·
2026
·Vol. 11
·期 32
·47638-47653
·
IF 5.2
Liu Yanchi,Sun Mohan,Qian Chengchao,Fu Yabo,Qiao Junwei,Wang Diangang,Shi Jiazi,Zhang Gaimei,Zhang Xinlin,Liu Hui
To overcome the poor
visible light response and high
recombination
rate of photogenerated carriers in bare TiO 2 , a Pt/Co 3 O 4 /TiO 2 photocatalyst was fabricated
via a template-assisted spontaneous galvanic replacement route. The
as-prepared material contains anatase–rutile mixed-phase TiO 2 , Co 3 O 4 , and metallic Pt and retains
a dodecahedral morphology with a high specific surface area of 122.64
m 2 /g. Under visible light irradiation for 120 min, its
degradation rates for tetracycline and methylene blue reached 85%
and 93%, respectively, which are significantly better than those of
pure TiO 2 and Pt/Co 3 O 4 . The composite
also exhibited excellent stability and recyclability. Its superior
performance is ascribed to the synergistic effects of the mixed-phase
TiO 2 , the p–n heterojunction between TiO 2 and Co 3 O 4 , the Schottky barrier at the Pt/TiO 2 interface, the localized surface plasmon resonance of Pt,
and the high adsorption capacity of the porous material. This work
offers a new strategy for treating dye- and antibiotic-containing
wastewater.
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ANALYTICAL AND BIOANALYTICAL CHEMISTRY
·
2026
·
IF 4.1
Wu Zejun,Ji Meiyu,Feng Sizhang,Zhang Xichun,Gan Ning,Zhao Cheng,He Jincan
The overuse of enrofloxacin (ENR) in aquaculture poses significant threats to ecological security and food safety, generating an urgent demand for instrument-free on-site detection. Herein, a Listeria -templated Ag-Pt bimetallic nanozyme ( Listeria -Ag@Pt) was fabricated via a bacteria-templated in situ mineralization strategy. The intact bacterial template not only prevents nanoparticle aggregation to maximize peroxidase-like activity but also imparts inherent molecular recognition capability toward ENR without requiring antibodies or aptamers. The presence of ENR can enhance the catalytic efficiency of the nanozyme, significantly accelerating the oxidation of 3,3′,5,5′-tetramethylbenzidine (TMB) by H 2 O 2 to produce blue oxTMB. Based on this target-enhanced chromogenic response, a colorimetric sensing platform was established, exhibiting a wide linear range of 0.0025–20 mg/L and a low limit of detection (LOD) of 0.8 ng/mL. The method afforded satisfactory recoveries of 92.7%–105% with relative standard deviations (RSDs) of 2.2%–7.3% in aquatic products. With advantages of cost-effectiveness, simplicity, and excellent anti-interference performance in complex matrices, this naked-eye detection strategy shows promising application prospect for on-site monitoring of ENR residues. Graphical abstract
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2025
·
IF 11.3
Qian Zhao,Xuxing Lu,Heyun Fu,Xiaolei Qu,Shourong Zheng,Dongqiang Zhu
Precisely tuning the surface properties of Pt active sites is of great importance for designing highly active catalysts used in the low-temperature catalytic oxidation of ethylene (C2H4). Herein, carbon doped Pt catalysts supported on SBA-15 (PtCx/SBA-15) were prepared by ethane (C2H6) heat treatment on SBA-15 supported Pt catalysts (Pt/SBA-15). Characterization results disclose that carbon atoms are successfully introduced in Pt particles, forming unique PtCx active sites. The PtCx active sites exhibit strong C2H4 adsorption and activation ability, enhanced hydrophobicity, and high catalytic activity for CO oxidation. As a result, PtCx/SBA-15 catalysts exhibit much higher C2H4 conversion and CO2 yield than Pt/SBA-15 catalysts at 0 °C. Particularly, 3PtCx/SBA-15 maintains 100% conversion of 50 ppm of C2H4 for more than 7 h and even displays 93.2% C2H4 conversion and 88.8% CO2 yield after 20 h of time-on-stream (TOS), exhibiting unprecedentedly prominent catalytic performance. This study provides a universal and efficient strategy to accurately enhance the surface hydrophobicity of noble metal particles employed in the low-temperature catalytic oxidation of C2H4. More importantly, it opens a new pathway for constructing highly active catalysts from the perspective of accelerating the oxidation of intermediate species to achieve improved utilization efficiency of active sites.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Lu Hao,Zhangyou Wang,Jiawen Li,Fangge Cheng,Jia Liu
Advancements in direct methanol fuel cells (DMFCs) have underscored the critical need for efficient electrocatalysts owing to sluggish methanol oxidation reaction (MOR) kinetics. The coupling of Au and Pt regulates Pt electronic structure, enhancing catalytic performance. To further optimize Pt catalytic performance and improve atomic utilization efficiency, we designed an active structure featuring heteronuclear Pt Au atomic pairs coupled with Pt clusters. By carefully controlling the sequence of key synthesis steps, we successfully developed the Pt@Pt-Au/NC-2 catalyst, achieving an optimal mass activity of 4.77 A mg Pt − 1 and specific activity of 4.57 mA cm − 2 , outperforming commercial Pt/C catalysts by 5.81- and 3.20-fold, respectively. Additionally, the catalyst demonstrates exceptional CO tolerance, ensuring excellent long-term stability. Experimental findings integrated with density functional theory (DFT) calculations demonstrate that the electronic effects of the atomic Pt Au pair enhance the CO oxidation rate and the synchronization of the hydroxide-mediated proton coupled electron transfer (HM-PCET) process, thereby facilitating the methanol oxidation reaction. This research not only emphasizes the precise synthesis of advanced atomically dispersed materials but also deepens the understanding of structure-performance relationships in multi-metallic catalytic systems, contributing to a wide range of its applications.
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Engineering
·
2025
·
IF 11.6
Chao Sun,Tianzuo Wang,Ruijie Gao,Xiaoyang Liu,Kang Xue,Chengxiang Shi,Xiangwen Zhang,Lun Pan,Ji-Jun Zou
Understanding the intrinsic features of dehydrogenation reactions of liquid organic hydrogen carriers (LOHCs) is a formidable challenge due to the combined impact of electronic and geometric effects. Herein, we constructed a series of Pt/MO x catalysts (CeO 2 , MgO, ZrO 2 , TiO 2 , Al 2 O 3 , or SiO 2 ) with similar sizes of Pt (∼1.7 nm) to investigate the effects of Pt electron structures (tuned by electronic metal‒support interactions) on the catalytic dehydrogenation of LOHCs. The results revealed a volcano-shaped correlation between Pt d electrons on different supports and the turnover frequency of catalytic dehydrogenation. Importantly, the Pt/MgO catalyst exhibited the highest dehydrogenation activity. With decreasing d electron content, Pt/MgO increases the bonding orbital dominance of Pt‒C bonds and leads to stable adsorption of H6-monobenzyltoluene (MBT), which facilitates subsequent C‒H bond scission. This study offers insight for the strategic development of high-efficiency dehydrogenation catalysts via d electron density modulation of Pt sites.
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CARBON
·
2025
·
IF 11.6
Ziyue Han,Wei Deng,Yujie Song,Hailiang Cao,Yongqing Shen,Zhijian Dang,Zhi Zheng,Junjie Guo
Carbon-supported platinum (Pt/C) is the most extensively used electrocatalyst for the oxygen reduction reaction (ORR). However, the electrochemical degradation occurring during operation severely restricts the catalyst's cycling stability, posing a critical obstacle for practical commercialization. Here, we developed a high-performance alternative electrocatalyst consisting of ultrafine Pt nanoparticles embedded in hierarchical porous carbon nanofibers (Pt/PCNF). Importantly, we elucidate a novel micropore confinement effect, demonstrating through DFT calculations that micropores serve as high-surface-area anchoring sites for Pt species, effectively stabilizing them. This unique architecture facilitates ultrahigh Pt dispersion, endowing the catalytic with exceptional stability for pH-universal ORR. Remarkably, the Pt/PCNF catalyst achieves 70 % higher electrochemically active surface area than commercial Pt/C while maintaining 99.4 % of its initial activity after 10,000 durability cycles. Furthermore, when integrated into Zn-air batteries, the catalyst delivers a high open-circuit voltage (1.42 V) and remarkable peak power density (216.73 mW cm −2 ). This work provides fundamental insights into the stabilization mechanisms of Pt-based ORR catalysts through micropore confinement, while demonstrating exceptional performance metrics that meet industrial requirements for fuel cell applications.
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ACS Catalysis
·
2025
·
IF 13.1
Yanfei Liu,Zhang Liu,Yi Yu,Chun Du,Jie Xu,YaoHui Dun,Chengxiong Wang,Yunkun Zhao,Aimin Zhang,Fudong Liu,Wei Li,Rong Chen,Bin Shan
Isolated atom catalysts face challenges in structure-sensitive reactions due to their oxidic electronic states and the lack of ensemble sites. A strategy employing the coupling between the coordination environment and adsorbate species is developed to overcome these limitations by constructing PtCu heteroatom ensembles, which unleashes the latent power of isolated Pt atoms for NH3–SCO reactions. Through the integrated exploration of theoretical calculations and experimental studies, we elucidate the pivotal role of structural sensitivity and isolated Pt coordination environments in shaping the electronic structure of Pt and its interaction with adsorbates. Our work reveals the Cu–Pt1–Cu atomic site as a breakthrough configuration, displaying unprecedented catalytic activity and selectivity in NH3–SCO reactions, far surpassing traditional Pt-based catalysts. Remarkably, the dispersed Cu–Pt1–Cu heteroatom ensemble achieves a turnover frequency of 0.29 s–1 at 150 °C, being the highest among Pt-based catalysts, and outperforming representative Pt1 SACs by an impressive 6 orders of magnitude, while its N2 selectivity remains above 89.7%. This heightened performance is attributed to its distinctive electronic properties, characterized by free-atom-like metallic Pt electronic orbitals embedded within a bulk like Pt1–Cun ensemble structure.
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MICROCHEMICAL JOURNAL
·
2026
·
IF 5.1
Meilin Liu,Yi Duan,Yiyao Luo,Xuhui Xia,Mingyi Guo,Danqun Huo,Changjun Hou
Ochratoxin A (OTA), a prevalent cereal mycotoxin, exhibits carcinogenic and teratogenic properties that threaten public health. Consequently, sensitive and reliable OTA detection methods are critically needed. A CRISPR-Cas12a-mediated colorimetric biosensor was developed, integrating Cas12a regulation via modular hairpin structures with MOF@Pt@MOF nanozyme amplification. Hairpin structures incorporate target-specific sequences; target binding induces rearrangement, preventing Cas12a recognition while enabling dsDNA activators to restore Cas12a function. Magnetic beads (MBs) were coupled with MOF@Pt@MOF nanozymes via ssDNA to construct MBs-MOF@Pt@MOF probes. Following OTA-induced activation, Cas12a cleaves ssDNA, releasing nanozymes into the supernatant, catalyzing TMB oxidation to generate a blue chromophore. A detection limit of 0.055 ng/mL was achieved with excellent selectivity. This approach utilizes inhibitory aptamer conformational changes for precise Cas12a regulation and nanozyme signal amplification to enhance sensitivity and specificity. The modular design demonstrates versatility for diverse target detection in point-of-care testing (POCT) applications.
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Journal of Materials Chemistry A
·
2026
·
IF 9.5
Wajeeha Fatima,Jie Chen,Jiujiang Zhao,Ning Zhang,Mengxin Xiao,Huiya Zhang,Qi Chen,Xiong Yin,Minghui Liang
This study demonstrates the separate manipulation of electronic and geometric effects in Pt-Co/C catalysts, where Co single atoms decorate Pt nanoparticles, to solve two issues in ECH selective hydrogenation: dechlorination and ring-opening regioselectivity. We decoupled these effects by synthesizing two model catalysts: Co/C-Pt (for electronic effect) and Pt/C-Co (for geometric effect). The electronic effect, characterized by XPS, enhanced the selectivity of 1-chloro-2-propanol from 80.1% to 96.7%. The geometric effect, confirmed by H₂-O₂ titration, drastically improved the yield of the anti-Markovnikov product (3-chloro-1-propanol) from 0.4% to 41.9%. Combined TPD and DFT calculations reveal that the Co atoms tailor the adsorption properties of Pt and the configuration of adsorbed ECH, which is the origin of the enhanced catalytic performance.
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