Journal of Materials Chemistry A
·
2026
·
IF 9.2
Chonghan Xia,Junhao Ma,Qihang Chen,Yee Yan Tay,Lydia H. Wong,Kwan W. Tan
The synthesis of ordered mesoporous multimetallic alloys (MMAs) with controlled composition remains challenging due to disparate reduction kinetics of multimetal precursors. Here we report a one-pot nanocasting approach in which PtFeCoNiCu salts are co-infiltrated and co-reduced within a gyroidal KIT-6 mesoporous silica scaffold, followed by template removal and acid etching, yielding single phase fcc mesoporous alloys with a 3D bicontinuous network morphology. By tuning the reduction conditions, we regulate the incorporation of Fe, Co and Ni around a PtCu-rich solid-solution lattice and remove FeCoNi overgrowths, exposing an ordered Pt-based mesoporous framework with excellent HER performance. The optimized ordered MMA catalyst, delivers an overpotential of 25 mV at 10 mA cm−2, a Tafel slope of 49.1 mV dec−1, and negligible degradation over 100 000 cycles, outperforming both commercial Pt/C and mesoporous Pt controls. This work demonstrates a general route to compositionally tuned ordered mesoporous multimetallic solid-solution alloys suitable for catalysis, sensing and related functional materials.
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Materials Science and Engineering B-Advanced Functional Solid-State Materials
·
2026
·
IF 5.7
Huijun Wang,Junhai Wang,Xi Chen,Chonghao Yang,Weibin Li,Qihao Jiang,Xingyu Zhan,Hongbin He,Naixu Li,Li Zhang,Jiancheng Zhou
Multicarbon fuel synthesis achieved via photothermal-photocatalytic coupling. • Localized thermal flux synergizes with charge dynamics to accelerate surface kinetics. • Pt loading minimizes carrier recombination and maximizes solar-to-chemical efficiency. The integration of photothermal and photocatalytic processes presents a promising pathway to boost solar-driven CO 2 conversion, yet achieving efficient photo–heat synergy under concentrated sunlight remains challenging. Here, we report a Pt-nanoparticle-decorated WO 3 catalyst fabricated via chemical reduction, which demonstrates exceptional activity for CO 2 reduction under concentrated solar irradiation. The optimized 0.8Pt/WO 3 catalyst achieves CO, CH 4 , and C 2 H 4 production rates of 4.12, 2.12, and 0.63 μmol·h −1 ·g −1 , respectively, with a noteworthy 25.8- and 28.3-fold enhancement in CO and CH 4 yields upon switching from unconcentrated to concentrated light. Systematic characterization reveals that Pt nanoparticles not only act as electron sinks to facilitate charge separation and interfacial transfer, but also enhance visible-light absorption and photothermal conversion. Under concentrated irradiation, the coupled photothermal effect elevates the local temperature to ∼405 °C, promotes high-density carrier accumulation, and significantly lowers the apparent activation energy from 21.21 to 13.80 kJ·mol −1 . This work elucidates a synergistic photothermal–photocatalytic mechanism where enhanced charge dynamics and localized heating jointly drive efficient CO 2 valorization, offering a design blueprint for high-performance solar fuel catalysts.
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Frontiers in Chemistry
·
2026
·
IF 5.3
Xing Li,Xiaonian Li
Carbon-encapsulated metal catalysts can have a high stability. The catalytic activation mechanism of the inert carbon shell requires further investigation. We prepared platinum-core carbon-shell catalysts on activated carbon supports. The graphitization degree of the carbon layer was tuned through pyrolysis temperature control. The catalysts were tested in the selective hydrogenation of p-chloronitrobenzene. The intact carbon shell physically isolates the metal core. All coated samples achieved a target product selectivity above 99%. The catalytic activity exhibited a distinct volcano trend. The sample treated at 800 °C delivered the highest activity. Experimental and theoretical analyses revealed an interfacial electron transfer process. The metal core acts as an electron pump to enrich the carbon surface. The optimal activity originates from a balance between electronic and geometric effects. The electron-rich surface lowers the hydrogen dissociation barrier. The preserved carbon defects serve as necessary adsorption sites. The core-shell structure suppressed metal sintering and the catalyst maintained good stability over 10 reaction cycles. This study provides a basic understanding for the design of highly active carbon-functionalized interfaces.
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Journal of Physical Chemistry C
·
2026
·Vol. 130
·期 31
·10958-10966
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IF 3.4
Li Wen-Tao,Zhang Cong-Cong,Deng Zheng-Dang,Feng Jing-Ru,Huang Fan,Ren Lin-Hao,Ding Si-Jing,Liu Xiao-Li,Ma Liang
Semiconductor-metal
heterostructured nanomaterials, featuring efficient
electron-transfer pathways, excellent light-harvesting capability,
and effective separation of photogenerated charge carriers, have emerged
as highly promising candidates for photocatalytic hydrogen production.
In this study, a thin Ag transitional layer was first deposited onto
the surface of Au NBPs, followed by growth to construct heterostructures
featuring pairwise interfacial contact among Au, Pt, and CdS. Morphological
and compositional characterizations reveal that Pt is located at the
tips of the Au NBPs and CdS grows at the midsection, resulting in
a unique heterostructure characterized by remarkably distinctive pairwise
contacts. Experiments show that the Au-Pt-CdS heterostructures exhibit
hydrogen-production efficiencies about 8 times higher than that of
Au-CdS heterostructures and approximately 223 times higher than that
of Au-Pt heterostructures, and also demonstrates excellent photocatalytic
stability. Owing to the work function difference between the metal
and the semiconductor, this heterostructure generates unique band
bending and an intrinsic electric field at the interface, effectively
facilitating the separation and multipath directional transport of
photogenerated charge carriers, thereby significantly enhancing the
rate of photocatalytic hydrogen evolution. Our study provides valuable
guidance for the rational design of high-efficiency semiconductor-metal
heterostructured photocatalysts and holds significant promise for
advancing low-carbon energy solutions and promoting sustainable societal
development.
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Small
·
2026
·
IF 11.8
Xuewen Xia,Fuqian Wang,Nannan Zhang,Li Tao,Xin Yuan,Xueqiang Zhang,Zhenqiang Jiang,Shujuan Wang,Xing Yu,Zhongya Pang,Guangshi Li,Xionggang Lu,Xingli Zou
Metal vacancies in MXene catalysts are beneficial for modulating electronic structures and enhancing metal-support interactions for single-atom (SA) immobilization, but controlling their concentration and understanding their synergy with SAs remains challenging. Here, we develop a two-step electrochemical etching strategy in a deep eutectic solvent to create tunable Ti vacancies within MXene (Ti V -Ti 3- x C 2 T y ) and confine Pt single atoms (Pt SA -Ti V -Ti 3- x C 2 T y ). The vacancy concentration is precisely controlled, and the dynamic etching-deposition process prevents Pt SAs aggregation. The resulting catalyst with only Pt content of 0.57 wt.% exhibits excellent alkaline hydrogen evolution reaction (HER) performance: an overpotential of 31 mV at 10 mA cm −2 , a turnover frequency of 12.22 H 2 s −1 , and a mass activity of 11.95 A mg Pt −1 at 100 mV, outperforming commercial Pt/C. The coexistence of Pt SAs and adjacent Ti vacancies synergistically tunes the local electronic structure of Pt sites and modulates metal-support bonding, lowering the water dissociation barrier and optimizing hydrogen adsorption energy to boost alkaline HER. This work offers a controllable strategy for engineering metal vacancies in MXenes for efficient single-atom catalysts and establishes a platform for investigating vacancy-SA synergistic mechanisms.
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Catalysts
·
2026
·Vol. 16
·期 8
·689
·
IF 4.5
Zhongqiang Bao,Yiwei Zhang,Zhenhua Ji,Zhenguo Li,Peng Zhang,Ding Luo,Zhanming Chen,Han Gao,Lei Zhu,Hao Chen
Supported Pt catalysts are highly active for the selective catalytic oxidation of ammonia (NH3-SCO), but their practical use is limited by poor N2selectivity and insufficient hydrothermal durability under high-temperature exhaust conditions. Herein, we report a composition-regulated high-entropy oxide interface strategy to stabilize Pt–Cu dual sites and steer NH3oxidation toward selective N2formation. A series of fluorite-type Ce-based high-entropy oxides, including CeZrLaPrYOx, CeSmLaPrYOx, and CeSnLaPrYOx, were constructed as thermally robust supports for Pt and Cu loading. Among them, PtCu/HEO-Zr calcined at 1000 °C exhibits the best NH3-SCO performance, achieving 90% NH3conversion at 260 °C while maintaining N2selectivity above 80% over a broad temperature window of 100–300 °C under a high weight hourly space velocity of 100,000 mL·g−1·h−1. More importantly, after harsh hydrothermal aging at 800 °C with 10 vol% H2O for 12 h, the catalyst shows negligible activity loss and nearly unchanged N2selectivity, demonstrating exceptional structural and catalytic robustness. Structural and surface analyses reveal that Zr incorporation optimizes the fluorite high-entropy lattice, increases oxygen vacancy concentration, promotes lattice oxygen mobility, strengthens surface acidity, and enriches active Cu2+species, thereby enhancing the interfacial cooperation between NH3activation and oxygen-assisted intermediate conversion. In situ DRIFTS further reveals that PtCu/HEO-Zr favors an Olat-assisted internal selective catalytic reduction pathway, in which adsorbed NH3is activated to -NH2species and subsequently reacts with lattice oxygen-derived intermediates to form N2O22−-like species that decompose into N2and H2O. Meanwhile, the formation of nonselective NOxand N2O products is suppressed. This work highlights high-entropy oxide-supported Pt–Cu interfaces as a promising platform for designing hydrothermally durable and N2-selective NH3-SCO catalysts.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2026
·
IF 6.7
Jiaxuan Cui,Xi Feng,Peng Peng,Tao Chen,Taiyu Zhou,Tianming Li,Li Zhang,An Xue,Zhanming Dou,Fangping Wang,Guifen Fan,Fangfang Zeng
To address the demand for high-precision piezoelectric devices featuring high piezoelectric performance and excellent temperature stability, x Ce-PMN-35PT piezoelectric ceramics were synthesized via cerium doping. Ce ions preferentially occupy the A-site substituting for Pb 2 + , as evidenced by XRD peak shifts and Raman spectral evolution. Combined lattice variation and ionic radius data suggest a valence evolution from Ce 4+ towards Ce 3+ with increasing doping content. The results show that the ceramic with 2 mol% Ce doping exhibits superior comprehensive performance: the piezoelectric coefficient d 33 reaches 780 pC/N, the large-signal piezoelectric coefficient d 33 * is 1101 pm/V, and the unipolar electrostrain only degrades by 6.4% across the broad temperature range from 25 to 125 ℃. Through in situ XRD and Rietveld refinement, this study further elucidated the intrinsic correlation among phase structure, domain switching dynamics, and piezoelectric properties, thereby revealing the underlying mechanism by which cerium doping optimizes material performance. This work not only offers a promising material system for medium-temperature high-precision piezoelectric actuators but also presents an effective strategy for tailoring the properties of PMN-PT-based ceramics.
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TALANTA
·
2026
·
IF 6.7
Xiao Wang,Kai Liu,Zhihao Qu,Kun Zhao,Fengran Zhang,Jun Wang,Xue Zhang,Weiliang Tian,Kewei Zhang
Ammonia (NH 3 ) leakage poses significant risks to industrial safety, environmental quality, and human health, highlighting the development of highly sensitive sensors operating at room temperature. Herein, ultrasmall platinum nanoparticles (Pt NPs, ∼2 nm) were confined within the ordered channels of conductive Cu 3 (HHTP) 2 metal-organic framework (MOF) via an in-situ reduction strategy to construct Pt@Cu 3 (HHTP) 2 nanocomposites. Benefiting from the spatial confinement effect, the Pt NPs were uniformly dispersed without disrupting the crystallinity of Cu 3 (HHTP) 2 , with Pt predominantly existing in metallic state (Pt 0 ). The resulting Pt@Cu 3 (HHTP) 2 sensor exhibited a high response of 142% toward 4 ppm NH 3 at room temperature, along with fast response and recovery times (124/68 s), and a low detection limit of 157 ppb. In addition, the sensor demonstrated excellent repeatability, long-term stability, and high selectivity against multiple interfering gases. The introduction of Pt NPs promotes oxygen adsorption and dissociation through synergistic chemical and electronic sensitization effects, thereby facilitating interfacial electron transfer and improving sensing performance. This work provides a rational strategy for engineering conductive MOF-noble metal composites and highlights their potential for reliable room-temperature NH 3 monitoring.
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DENTAL MATERIALS
·
2026
·
IF 6.3
Meng Bo,Jiao Fang,Yuning Wu,Zixuan Chen,Yingchi Liu,Shuang Liu,Chunyan Li,Lin Wang,Xiaolin Sun
A metabolically reprogrammed MnO₂-Mg/Pt@BBF nanozyme is developed for periodontitis treatment. • Mg²⁺ amplifies endogenous H₂O₂ production via SpxB in Streptococcus gordonii. • Pt decoration enriches catalytically active Mn²⁺ to enhance chemodynamic therapy. • Covalently immobilized BBF inhibits LuxS/AI-2 quorum sensing and disrupts biofilm cohesion. • The nanozyme reduces bacterial burden, alveolar bone loss, and inflammation in vivo . Objectives To overcome the intrinsic incompatibility between dense periodontal biofilms and chemodynamic therapy (CDT), we developed a vacancy–engineered MnO₂ nanozyme that integrates redox–state programming, Mg²⁺–enabled endogenous H₂O₂ amplification, and covalently immobilized quorum–sensing inhibition for the local treatment of periodontitis. Methods Mg²⁺–coordinated MnO₂ nanoflowers were decorated with Pt nanoparticles and covalently functionalized with BBF. Physicochemical properties, Mn valence states, H₂O₂ and ·OH generation, LuxS/AI–2 signaling, Porphyromonas gingivalis metabolomic changes, antibiofilm activity, and therapeutic efficacy in rat periodontitis were evaluated. Results Pt decoration increased the Mn²⁺ fraction from 33% to 51%, while Mg²⁺ enhanced SpxB–mediated H₂O₂ production by Streptococcus gordonii . Immobilized BBF reduced AI–2 activity from 67.8% to 22.8% and downregulated luxS, fimA, mfa1, kgp, and rgpA . In dual–species biofilms, MnO₂–Mg/Pt@BBF yielded 68.7% dead cells, an approximately 4–log₁₀ reduction in viable bacteria, and the lowest residual thickness. Metabolomics revealed depletion of G6P, R5P, NADPH, ATP, and α–ketoglutarate in P. gingivalis. In vivo , treatment reduced periodontal bacterial burden by approximately 3 orders of magnitude and decreased the CEJ–ABC distance from 1.44 ± 0.28 mm to 0.56 ± 0.15 mm, accompanied by reduced inflammation and IL-6 expression, improved collagen organization, and elevated Arg-1 levels. Significance This locally deliverable platform couples vacancy/valence–tuned catalysis, Mg²⁺–primed endogenous oxidant supply, and surface–immobilized quorum–sensing blockade, offering a composition–guided strategy for controlling polymicrobial periodontal biofilms and limiting infection–associated tissue destruction.
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ACS Nano
·
2026
·
IF 17.3
Shanli Wang,Zejin Ju,Yingwu Wang,Zijie Liu,Xingzhe Wang,Hua Jiao,Minhua Cao,Yude Wang,Wenyan Yin,Yuliang Zhao
Nanozymes suffer from insufficient catalytic activity and sluggish electron transfer, while hypoxic tumor microenvironment (TME)-induced radioresistance and limited reactive oxygen species accumulation hinder radiotherapy efficacy. Existing nanozyme radiosensitizers often require high-dose radiotherapy or combined drugs to achieve only a modest efficacy. Herein, we report a Pt-anchored MoOx (MPP) nanozyme synthesized via a surface defect-ligand reduction strategy with Pt nanoclusters loading up to 34.39 ± 0.92 wt %. It features a gradient electron-transfer interface constructed by strong Pt–O–Mo interactions, which enables atomic-level integration of Pt0/Pt2+ nanoclusters with MoOx and the simultaneous introduction of oxygen vacancies and an interfacial electron pool. Density functional theory calculations confirm the interface upshifts MoOx’s d-band center, accelerates Mo → Pt electron transfer, and reduces the H2O2 dissociation barrier to 0.18 eV. Consequently, MPP achieves a catalase-like specific activity of 3884.53 U mg–1 (2-fold natural catalase, 7528-fold MnO2) and a turnover number (TON) of 25.7021 s–1. Additionally, MPP exhibits a quantitative factor for electron transfer efficiency of 1.75, exceeding reported nanozymes. In the acidic TME, MPP orchestrates a catalase/superoxide dismutase/oxidase cascade to relieve hypoxia and generate •O2–/1O2. Synergized with Pt’s high-Z effect, MPP amplifies the efficacy of 6 Gy with low-dose radiotherapy, achieving 75.24% tumor inhibition rate without inducing systemic toxicity. This gradient electron-transfer interface strategy provides a promising paradigm for high-efficacy, low-toxicity tumor-specific therapy.
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ACS Catalysis
·
2026
·
IF 13.6
Yu-Jun Xu,Chiao-An Hsieh,Chen-Yu Zhang,Li-Dan Zhang,Han Tang,Lu-Lu Zhang,Jun Cai,Yan-Xia Chen,Shuehlin Yau,Zhi-Feng Liu
Electrochemical energy and substance conversion devices involve complex electrode processes characterized by multiple charge transfer steps, competing pathways, and various intermediates. Such complexity makes it challenging to enhance the electrocatalytic activity. The prevailing strategy typically focuses on optimizing the geometric and electronic structures of the electrocatalysts to align the adsorption energies of reaction intermediates with the peak of the activity Volcano curve. In this study, we demonstrate that surface decoration can effectively shape the micro reaction environment for the model system of the oxygen reduction reaction (ORR) on Pt electrodes. By applying a partial hydrophobic I* adlayer on the Pt surface, we can shift the equilibrium of OH* reduction and weaken H2O* adsorption, which significantly enhances ORR kinetics. With in situ scan tunneling microscopy (STM) and theoretical calculations, our study reveals the formation of isolated Pt2 surface units situated in a hydrophobic valley surrounded by adsorbed iodine atoms. This minimalist Pt2 active unit exhibits significantly greater activity for the ORR compared to an extended Pt surface. Our results overturn the previous consensus that the I* adlayer always poisons the electrocatalytic reaction. Our systematic studies also reveal that whether I* acts as a poison or a promoter, as well as the extent of its promotional effect, depends on its coverage. This finding could pave the way for developing highly efficient catalysts with potential applications in fuel cell technology and metal air batteries and extension to other electrochemical conversion reactions such as ammonia synthesis and CO2 reduction.
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ACS Nano
·
2026
·
IF 17.3
Yaming Liu,Zhenle Hu,Xinrui Zhu,Xinyu Li,Tong Zuo,Yutian Zhao,Guoqiang Liu,Yanting Cheng,Chao Zhi,Jiaguang Meng,Xiang Li,Jingnan Wang,Mingshang Jin
While traditional Pt-based catalysts suffer from inadequate selectivity and stability in electrocatalytic ethylene glycol oxidation reactions, we present a general and scalable synthesis strategy, fabricating a broad multimetallic Pt-based alloy nanowires (NWs) library from binary to quinary. Among these, the PtAgCuRhRu NWs exhibit exceptional performance, with a mass activity ∼8 times higher than that of Pt/C and a Faradaic efficiency for glycolic acid (GA) reaching 93.49%. In the membrane electrode assembly electrolyzer, the catalyst maintained its activity over 140 h with 99% GA selectivity. In situ experimental and theoretical calculations reveal oxygenophilic Rh and Ru promote *OH adsorption, facilitating the conversion of *COCH2OH to GA and the oxidative removal of COads, enhancing activity and stability. Additionally, the high energy barrier for C–C bond cleavage suppresses undesired decomposition due to the introduction of Ag and Cu, leading to superior GA selectivity.
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