ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Qi Zhong,Kangdong Wang,Gao Pan,Shuping Peng,Cijun Shuai
CeO2 nanozymes have demonstrated the potential to enhance biological scaffolds with chemodynamic therapy. However, their catalytic efficacy is limited by the slow conversion of Ce4+ to Ce3+ and the lack of substrates like H2O2 and H+. To address these challenges, we adopted a dual-pronged strategy that utilized the plasmonic resonance of Au nanoparticles and their glucose-oxidase mimicry to boost electron and hydrogen transfer. Specifically, we integrated Au/CeO2 nanozymes into poly-l-lactic acid scaffolds via selective laser sintering. This conversion of Ce3+ to Ce4+ in the scaffolds enhanced the reduction of H2O2 to a hydroxyl radical, inducing oxidative stress in tumor cells. The Au nanoparticles played a crucial role in boosting the Ce3+/Ce4+ catalytic cycle by providing both the energy and the catalytic substrates. They recycled Ce4+ back to Ce3+ by exploiting plasmonic-induced hot electrons and catalyzed glucose oxidation to supply H2O2 and H+. Our nanoscale and atomic-scale simulations confirmed that the Au/CeO2 hybrid structure utilized near-field coupling to amplify the plasmonic resonance and the Au–O–Ce bridge reduced the electron transfer barrier. Consequently, the Au/CeO2 scaffold decreased the activation energy from 22.57 to 9.92 kJ/mol. These findings highlight the significant promise of the Au/CeO2 nanozyme scaffold for NIR-enhanced chemodynamic therapy.
研究领域:
纳米技术
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癌症治疗
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材料科学
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生物医学工程
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高影响因子
Nature Communications
·
2025
·Vol. 16
·期 1
·1-12
·
IF 15.7
Song Hui,Sun Kai,Huang Hengming,Ning Shangbo,Wang Shengyao,Wang Zhuan,Weng Yuxiang,Cui Yi,Li Yifan,Wang Xu-sheng,Wang Defa,Liu Lequan,Wang Zhou-jun,Ye Jinhua
The direct photocatalytic oxidation of methane to value-added chemicals has garnered considerable interest in recent years. However, achieving high productivity while maintaining high selectivity at an appreciable methane conversion rate remains a formidable challenge. Here, we present photochemically-triggered and photothermally-enhanced oxidative coupling of methane to multi-carbon C 2+ alkanes over an Au and CeO 2 nanoparticle-decorated ZnO photocatalyst, which exhibits a record-breaking C 2+ production rate of 17,260 μmol g −1 h −1 with ~90% C 2+ selectivity under wide-spectrum light irradiation without a secondary source of heating. Comprehensive characterizations and computational studies reveal that CH 4 activation is a photochemical reaction initiated by ultraviolet light-excited ZnO, and the introduction of CeO 2 substantially enhances the activation of CH 4 and O 2 due to the cooperative interaction between Au and CeO 2 . Concurrently, Au nanoparticles capture visible and near-infrared light to generate localized heating, which greatly promotes the subsequent desorption of produced methyl radical for C–C coupling prior to undergoing further undesired overoxidation.
研究领域:
化学工程
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材料科学
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环境科学
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JOURNAL OF ENVIRONMENTAL MANAGEMENT
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2025
·
IF 8.4
Junzi Huang,Mengjie Lu,Min Liu,Yahong Xie,Peng Wei,Huihui Xie,Liang Li,Weitao Han,Zhiwei Zhang,Ying Qi
The residues of tetracyclines (TCs) antibiotics present significant challenges in terms of contamination and pose a threat to human health. In this study, a cost-effective n-type semiconductor, CeO 2 , were loaded with small amounts of Au nanoparticles were fabricated by one-step hydrothermal method under alkaline conditions in the presence of the surfactant CTAB. Characterization tests revealed that Au/CeO 2 had significant visible light absorption capacity and good e − /h + separation efficiency. Photocatalytic degradation results of TC showed that 2% Au/CeO 2 -CTAB had the highest photocatalytic activity, achieving a degradation rate of 86.4% within 90 min. These values were 3.8 and 2.6 times higher than those of pure CeO 2 and CeO 2 -CTAB (without Au loading), respectively. Loading Au nanoparticles substantially increased the visible light absorption range, reduced bandgap width, and lowered photo-generated carrier recombination rate. Residual e − /h + on the semiconductor surface activating functional groups, further promoting photocatalytic degradation of pollutants such as TC. Au-loaded CeO 2 nano-photocatalysts have potential applications in the environments polluted by antibiotic residues.
研究领域:
环境科学
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材料科学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Hongpeng Liu,Zhongliang Cao,Siyuan Yang,Zejian Dong,Zi-An Li,Xing Chen,Langli Luo
The dynamic behavior of oxide-supported metal catalyst interfaces under thermal and gaseous activation critically determines their catalytic performance. Using in situ TEM, we reveal the atomic-scale evolution of Au nanoparticles on CeO 2 supports during thermal treatment. The Au/CeO 2 interface structure depends on three key factors: epitaxial matching, nanoparticle morphology, and metal-support interactions, all governed by the balance between Au surface energy, cohesive energy, and interfacial energy with CeO 2 . Thermal activation induces significant structural reorganization in Au nanoparticles, exhibiting size- and support-dependent facet reorientation that follows temperature-driven wetting and sintering trends. These transformations are facilitated by crystalline defects (e.g., twin boundaries and dislocations) that reduce the energy barrier for atomic rearrangement.
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ACS Sensors
·
2026
·
IF 9.1
Lulu Tian,Songtao Hu,Qihang Ding,Zhenyu Ma,Cong Chen,Chunyan Li,Kun Wang,Juanrui Du,Yujia Shi,Jong Seung Kim,Lin Wang,Biao Dong
Monolayer noble metal nanoparticle (NP) arrays hold great promise as surface-enhanced Raman scattering (SERS) substrates due to their strong SERS performance and cost-effectiveness. However, precise regulation of hotspot intensity and density remains a critical challenge for practical applications. Here, we propose a SERS substrate based on Janus-structure NPs, which realizes accessible metal–semiconductor interface hotspots, as well as the regulation of interparticle nanogaps of ∼1 nm through a multifunctional surface ligand. By selectively depositing cerium oxide (CeO2) onto one terminus of gold nanorods (Au NRs), we fabricate Janus nanostructures that generate highly accessible and intensified hotspots. Another key enabler of this advancement is 4-mercaptophenylboronic acid (MPBA), a multifunctional ligand that precisely regulates interparticle spacing, increases hotspot density, and simultaneously serves as both a Raman molecule and a bacterial recognition unit. The SERS enhancement effect of the Janus NP array can reach more than 11 times that of the conventional Au NR array. Based on this MPBA-functionalized Janus NP array substrate, a SERS sensor for Escherichia coli was constructed, which exhibited a robust linear detection response to bacterial concentrations ranging from 6 to 6 × 104 CFU/μL, with an ultralow detection limit of approximately 1.1 CFU/μL. Our work introduces a versatile strategy for next-generation SERS substrates.
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NANO
·
2026
·
IF 1.3
Runcai Xu,Jiqing Dong,Xintao Gao,Xin Cheng,Xiangyan Chen,Yantao Li
Developing highly sensitive and stable nonenzymatic glucose sensors remains crucial for reliable glucose monitoring. Herein, we report an SMSI-driven Au/CeO 2 -BTC nanozyme derived from a Ce-BTC metal-organic frameworks (MOFs) for efficient electrochemical glucose detection. The Ce-trimesic acid (Ce-BTC) precursor was calcined to generate a porous CeO 2 -BTC framework with abundant oxygen vacancies, followed by the in situ deposition of Au nanoparticles. Structural analyses reveal the formation of Au-O-Ce interfacial sites, indicating pronounced trong metal-support interactions (SMSI) that induce electronic modulation, increase Ce 3+ concentration, and facilitate rapid charge transfer. Benefiting from these synergistic effects, the Au/CeO 2 -BTC-modified electrode exhibits excellent catalytic activity toward glucose oxidation, achieving a sensitivity of 41.3 µA cm -2 mM -1 and a detection limit of 4.75 µM, along with good reproducibility, stability, and selectivity. This work highlights the importance of SMSI engineering in MOF-derived nanozymes and provides an effective strategy for constructing high-performance electrochemical glucose sensors
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INORGANIC CHEMISTRY
·
2025
·
IF 4.7
Bin Zhang,Shuo Liu,Hao Deng,Ye Pei,Qingxue Mu,Yuming Lei,Taolei Sun,Guanbin Gao
Plasmonic metal and semiconductor heterostructures have recently emerged as a promising strategy to enhance the rate of catalyzed reactions. However, most research has predominantly focused on plasmon-induced hot electron transfer mediated by localized surface plasmon resonance (LSPR), while the photothermal effects of plasmonic metals have been largely underexplored. In this study, a dumbbell-shaped Au nanobipyramids (AuNBPs)/CeO2 heterojunction with superior photothermal properties was designed as a catalytic platform for the hydrolysis of organophosphorus compounds and the reduction of 4-nitrophenol (p-NP). The results demonstrated that the photothermal effect at the interface between AuNBPs and CeO2 is the dominant mechanism accelerating the reaction. Moreover, for the hydrolysis product p-NP, AuNBPs@CeO2 further converted it into 4-aminophenol (p-AP) in the presence of NaBH4, effectively preventing secondary pollution. In summary, the integration of AuNBPs with photothermal properties and CeO2 successfully achieved cascade catalytic degradation of organophosphates.
研究领域:
材料科学
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环境科学
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化学
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APPLIED ORGANOMETALLIC CHEMISTRY
·
2024
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IF 3.7
Xiaohua Zhao,Xiaoxiao Liu,Xiang Liu,Weiyi Li,Ping Wang
Integration of localized surface plasmon resonance (LSPR) metallic nanocrystals into photocatalysis is an intriguing approach for light-driven organic transformations. However, uncertain direction of hot carriers is a grand challenge, which fails to take full advantage of the LSPR excitation. In this work, core–shell gold@ceria nanosphere–supported segregated palladium species (Au@CeO 2 –Pd) have developed to steer the light absorption capability and charge carrier migration. Under simulated solar light irradiation, the core–shell–satellite Au@CeO 2 –Pd exhibited efficient light harvesting and colossal activity in the Suzuki coupling reaction. The plasmon-induced hot electrons overpassed the Schottky barrier at the Au@CeO 2 interfaces and migrated from Au core to CeO 2 shell accordingly. Subsequently, the photogenerated electrons and hot electrons migrated from Au@CeO 2 core–shells to Pd, which acted as an electron acceptor. Detailed photocatalytic mechanism studies revealed that both photoexcited electrons and holes were the main active species involved in the photocatalytic Suzuki coupling reaction process. In particular, the diphenyl yield over Au@CeO 2 –Pd catalyst was ~1.7 times higher than that of core–shell–satellite Au@SiO 2 –Pd, where a 19-nm-thick SiO 2 shell was introduced to prevent the migration of hot electrons. This distinctly certified that the hot electrons transfer in the core–shell–satellite Au@CeO 2 –Pd under illumination played an important role to drive Suzuki reaction. Overall, this design of core–shell–satellite Au@CeO 2 –Pd plasmonic photocatalyst has the potential in the field of photo-driven organic transformations.
研究领域:
材料科学
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化学工程
·
光化学
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高影响因子
CATALYSIS COMMUNICATIONS
·
2019
·
IF 3.674
Cuncun Zuo,Yun Tian,Yanxia Zheng,Lei Wang,Zhongjun Fu,Tiantian Jiao,Ming Wang,Haofei Huang,Yuchao Li
Series of gold and ceria supported γ-Al 2 O 3 catalysts were developed for the oxidative esterification of methacrolein with methanol. All the catalysts were prepared through one step deposition-precipitation method, and K 2 CO 3 and urea were used as precipitant, respectively. Au, CeO 2 and γ-Al 2 O 3 could self-assemble unique particle morphology during co-precipitation process and form semi-core shell or core shell structure after calcination . The relationship between catalytic reactivity and structural characteristics were analyzed by SEM, TEM, EDS, BET, XRD, XPS, etc. Among Au-CeO 2 /γ-Al 2 O 3 (K 2 CO 3 ), Au-Ce/γ-Al 2 O 3 (Urea) and Au/γ-Al 2 O 3 (Urea) catalysts with different active components and precipitant, the last two exhibited higher catalytic activity. Moreover, the Ce-doped catalysts shown higher stability than just Au supported on pure alumina. The active stability of the optimum Au-Ce/γ-Al 2 O 3 catalyst was evaluated with seven-time cyclic reactions exhibiting high stability and activity with the yield of MMA above 90%.
研究领域:
催化化学
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材料科学
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高影响因子
CANADIAN JOURNAL OF CHEMICAL ENGINEERING
·
2019
·Vol. 98
·期 3
·767-774
·
IF 1.61
Yuchao Li,Yun Tian,Yanxia Zheng,Tingting Ge,Zhongjun Fu,Tiantian Jiao,Ming Wang,Haofei Huang,Cuncun Zuo
A series of Zr-doped CeO 2 nanorods supported by Au nanoparticle catalysts with different morphologies were prepared for methyl methacrylate (MMA) synthesis via direct oxidation esterification of methacrolein (MAL) with methanol. Catalytic activities under mild conditions (0.3 MPa; 80°C) were evaluated in the kettle reactor. Different characterization methods, such as XRD, Raman, N 2 adsorption, ICP, TEM, SEM, XPS, and H 2 -TPR techniques, were applied to study the relationship between catalytic activity and structural characteristics, especially the form of Zr doped into the lattice of CeO 2 and the promotion mechanism of selective oxidation. The influence of Au supported on Ce 0.6 Zr 0.4 O 2 nanorods (Au/CZ-R) was also discussed. The results exhibited that the highest catalytic activity for the oxidative esterification with a MAL conversion of 99% and a MMA selectivity of 74% was achieved. The MMA synthesis performance correlated well with the surface oxygen vacancies, in particular for the active oxygen species around the Au particles.
研究领域:
催化化学
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材料科学
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ChemSusChem
·
2021
·Vol. 15
·期 13
·e202101983
·
IF 8.928
Yanan Wei,Yunlei Zhang,Yao Chen,Fang Wang,Yu Cao,Wen Guan,Xin Li
Graphical Saving face : Catalytic performance of Au/CeO 2 with different exposed CeO 2 crystal faces for oxidation of 5-hydroxymethlfurural to 2,5-furandicarboxylic acid is dependent on the oxygen vacancy (V O ) concentration. Higher V O concentration of Au/rod-CeO 2 (110) is more beneficial for adsorption of oxygen and formation of active oxygen species than Au/cube-CeO 2 (100) and Au/oct-CeO 2 (111). Developing an efficient catalyst to upgrade 5-hydroxymethylfurfural (HMF) to high-value-added downstream chemicals is of great significance in biomass conversion. Nanorod (110)-, nanocube (100)-, and nanooctaheron (111)-CeO 2 -supported Au nanoparticles were prepared to investigate the intrinsic effect of CeO 2 crystal faces on the oxidation of HMF to 2,5-furandicarboxylic acid (FDCA). The experimental results and density functional theory calculation revealed that the concentration of oxygen vacancy (V O ) for exposed specific crystal faces was crucial to the oxygen adsorption ability, and Au/nanorod-CeO 2 with the highest V O concentration promoted the formation of more oxygen active species (superoxide radical) on CeO 2 (110) crystal face than (100) and (111) crystal faces. Besides, the higher V O concentration could provide a strong adsorption ability of HMF, greatly boosting the activation of HMF. Thus, these results led to a superior catalytic activity for HMF oxidation over Au/nanorod-CeO 2 (FDCA yield of 96.5 %). In-situ Fourier-transform (FT)IR spectroscopy uncovered the HMF oxidation pathway, and the possible catalytic mechanism was proposed. The deep insight into the role of regulation for crystal faces provides a basis for the rational design of highly active facets for the oxidation of HMF and related reactions.
研究领域:
催化化学
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材料科学
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生物质转化
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高影响因子
JOURNAL OF CATALYSIS
·
2017
·
IF 6.844
Benxia Li,Baoshan Zhang,Shibin Nie,Liangzhi Shao,Luyang Hu
Exploiting photocatalysts with improved properties for solar-driven chemical reactions is of great significance in developing green chemistry. Here, a series of Au/CeO 2 hybrid nanofibers with different Au loadings have been fabricated by a simple method of electrospinning followed by calcination in air. The particle size and plasmonic absorption of Au nanoparticles (NPs) loaded in the nanofibers were analyzed and found to vary with the dosage of chloroauric acid in the precursor solution. The Au/CeO 2 hybrid nanofibers were used as photocatalysts for selective oxidation of benzyl alcohol to benzaldehyde with O 2 under simulated sunlight and visible light (>420 nm), respectively. The results showed that introducing Au NPs into CeO 2 nanofibers induced a great improvement in photocatalysis. The degree of improvement increased first and then decreased with the increase in Au loading, reaching an optimal level over 0.5 wt.% Au-loaded CeO 2 nanofibers. The photocatalytic reaction presents a very high selectivity of 100% for benzaldehyde, which is important for organic synthesis. The transient photocurrent responses of the Au/CeO 2 catalysts were also tested for corroborative evidence. After detailed discussion of various factors including plasmonic absorption, charge transfer, and surface activity of the photocatalyst, a possible mechanism for the photocatalytic oxidation of benzyl alcohol occurring at the Au–CeO 2 interface was proposed.
研究领域:
材料科学
·
化学工程
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高影响因子
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