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学者姓名:庄赞勇
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Single-atom catalysts (SACs) anchored on defective supports offer exceptional catalytic efficiency but face challenges in stabilizing isolated metal atoms and optimizing metal-support interactions. Here, a defect-driven strategy is reported to construct a 3D dendritic SAC comprising interwoven ultrathin TiO2 nanowires (NWs) with abundant oxygen vacancies (OVs) that stabilize atomically dispersed cobalt (Co) sites. Using hydrothermal synthesis followed by acid etching and calcination, Ti & horbar;Co & horbar;Ti motifs are engineered at OVs site. The 3D architecture provides multiscale porosity and charge transport, achieving syngas production rates of 28.4 mmol g(-1)h(-1) (CO) and 13.9 mmol g(-1)h(-1) (H-2) with a high turnover frequency (TOF) of 10.6 min(-1), surpassing many other state-of-the-art Co-based SACs. In situ Raman and electron paramagnetic resonance (EPR) analysis reveal OVs consumption during Co anchoring, while density functional theory (DFT) validates charge redistribution from Ti to Co, enabling efficient electron transfer and inducing strong electronic interactions that enhance CO2 adsorption and activation. The results highlight the interplay between atomic-scale coordination environments and macroscale architectural order in harnessing the catalytic potential of SACs and ultrathin 1D NWs.
Keyword :
CO2 photoreduction CO2 photoreduction defect engineering defect engineering oxygen vacancy oxygen vacancy single atom catalyst single atom catalyst ultrathin 1D nanowires ultrathin 1D nanowires
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GB/T 7714 | Yan, Jiawei , Lin, Yalan , Lin, Mingxiong et al. Defect-Driven Atomic Engineering: Oxygen Vacancy-Stabilized Co Single Atoms on Ordered Ultrathin TiO2 Nanowires for Efficient CO2-to-Syngas Photoreduction [J]. | SMALL , 2025 . |
MLA | Yan, Jiawei et al. "Defect-Driven Atomic Engineering: Oxygen Vacancy-Stabilized Co Single Atoms on Ordered Ultrathin TiO2 Nanowires for Efficient CO2-to-Syngas Photoreduction" . | SMALL (2025) . |
APA | Yan, Jiawei , Lin, Yalan , Lin, Mingxiong , Huang, Xinlian , Dong, Weilong , Huang, Haoyang et al. Defect-Driven Atomic Engineering: Oxygen Vacancy-Stabilized Co Single Atoms on Ordered Ultrathin TiO2 Nanowires for Efficient CO2-to-Syngas Photoreduction . | SMALL , 2025 . |
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Herein, a versatile amorphous-to-crystalline transformation (ACT) strategy is described, to furnish various metals (Cu, Co, Ni, Cs, and Y) based atomically dispersed catalysts (ADCs) on thin holey 2D Al2O3. This approach, which involves adjusting reactant stoichiometry, enables the continuous modulation of particle size of ADCs at an atomical level, giving the ultrafine products as single atom, cluster, or nanoparticle catalysts. This synthesis method allows a straightforward analysis and comparison of the reactivity of the ADCs catalysts based on the dispersion of the active metal. In the case of Cu, the cluster catalyst 0.2-Cu/Al2O3 outperforms the single atom catalyst 0.1-Cu/Al2O3 and the nanoparticle catalyst 0.3-Cu/Al2O3 in the oxidation of refractory organic molecules, thanks to its superior electron transport and surface adsorption properties. These findings are well supported by the Density functional theory (DFT) calculations. Additionally, this method facilitates the preparation of atomic clusters with a very small size of 0.5-1 nm, composed of just a few atoms, as exemplified by Ni-based ADCs. The developed synthesis enriches the library of ADCs and demonstrates the potential of amorphous-to-crystalline transformation in creating advanced ultrasmall functional materials.
Keyword :
amorphous-to-crystalline transformation amorphous-to-crystalline transformation atomically dispersed catalysts atomically dispersed catalysts cluster, precise size tailoring cluster, precise size tailoring single atom single atom
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GB/T 7714 | Wang, Yaping , Zhang, Tingshi , Huang, Xinlian et al. Amorphous-to-Crystalline Transformation for Tunable Synthesis of Single Atom, Cluster, and Nanoparticle Catalysts: Dispersion of Metal Elements (Cu, Co, Ni, Y, Cs) on Holey 2D Ultra-Thin Al2O3 Nanosheets [J]. | SMALL METHODS , 2025 . |
MLA | Wang, Yaping et al. "Amorphous-to-Crystalline Transformation for Tunable Synthesis of Single Atom, Cluster, and Nanoparticle Catalysts: Dispersion of Metal Elements (Cu, Co, Ni, Y, Cs) on Holey 2D Ultra-Thin Al2O3 Nanosheets" . | SMALL METHODS (2025) . |
APA | Wang, Yaping , Zhang, Tingshi , Huang, Xinlian , Zeng, Yurong , Wei, Siyuan , Zhuang, Zanyong et al. Amorphous-to-Crystalline Transformation for Tunable Synthesis of Single Atom, Cluster, and Nanoparticle Catalysts: Dispersion of Metal Elements (Cu, Co, Ni, Y, Cs) on Holey 2D Ultra-Thin Al2O3 Nanosheets . | SMALL METHODS , 2025 . |
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Heterojunction photocatalysts, which consist of two or more semiconductors, have garnered significant attention owing to their extensive benefits, including a broad-spectrum response, efficient carrier separation and migration, as well as robust redox capabilities. Among the myriad of semiconductors, graphitic carbon nitride (g-C3N4) and zinc indium sulfide (ZnIn2S4) have been extensively researched due to their low toxicity, straightforward and scalable synthesis processes, controllable microstructures, and exceptional chemical stability. Recently, there has been a trend towards integrating these two semiconductors to complement each other's strengths. Consequently, a systematic summary and outlook on g-C3N4/ZnIn2S4 heterojunction photocatalysts is both urgent and valuable. This review summarizes the advancements in the g-C3N4/ZnIn2S4 heterojunctions in the last 10 years. We first analyzed the charge-transfer mechanisms in the type-I, type-II, Z-scheme and S-scheme heterojunctions. Then the typical synthesis methods employed for creating g-C3N4/ZnIn2S4 heterojunctions are introduced. Subsequently, we delve into the regulation strategies for g-C3N4/ZnIn2S4 heterojunctions, including morphology optimization, heteroatom doping, defect engineering, and the construction of multinary composites. The design concept and superiorities of these strategies are thoroughly discussed. Following this, we systematically showcase the photocatalytic applications of g-C3N4/ZnIn2S4 heterojunctions, encompassing CO2 reduction, H2 evolution, pollutant degradation, H2O2 production, biomass conversion, photoelectrochemical sensors, and so forth. Last, we propose the challenges that lie ahead in future research endeavors. This comprehensive review is expected to provide an instructive guideline for rational design and applications of g-C3N4/ZnIn2S4 heterojunctions.
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GB/T 7714 | Lu, Yongjun , Zhuang, Zanyong , Li, Lingyun et al. Advancements and challenges in g-C3N4/ZnIn2S4 heterojunction photocatalysts [J]. | JOURNAL OF MATERIALS CHEMISTRY A , 2025 , 13 (7) : 4718-4745 . |
MLA | Lu, Yongjun et al. "Advancements and challenges in g-C3N4/ZnIn2S4 heterojunction photocatalysts" . | JOURNAL OF MATERIALS CHEMISTRY A 13 . 7 (2025) : 4718-4745 . |
APA | Lu, Yongjun , Zhuang, Zanyong , Li, Lingyun , Chen, Fei-Fei , Wei, Peishu , Yu, Yan . Advancements and challenges in g-C3N4/ZnIn2S4 heterojunction photocatalysts . | JOURNAL OF MATERIALS CHEMISTRY A , 2025 , 13 (7) , 4718-4745 . |
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Overcoming the challenges of integrating disparate components in nanoarchitectures, this study introduces a straightforward strategy based on a mixed-valence coordination approach, creating an ordered ternary heterostructure integrated with ultrasmall homojunction. This singular ordered homojunction-heterostructure unites ultrathin 1D rutile TiO2 nanowires (NWs) and ultrathin anatase TiO2 NWs with 0D Prussian Blue Analogs (PBAs) nanoparticles (NPs), all exhibiting crystallographic oriented alignment with each other, forming a ternary mesocrystals. Experimental and theoretical insights disclose that the complex interplay between these dissimilar components is governed by a spontaneous lattice match effect, which not only optimizes but also directs the charge transfer, thereby enhancing both efficiency and stability. It also allows for tailoring the valence states of Fe within the PBA, fine-tuning of the composite's photochromic properties, and introducing abundant defect structures that foster strong interaction with oxygen molecules, enabling controllable color-switching dynamics. Consequently, the FeII1-xFeIIIx-PBA/TiO2 exhibits an optimized ternary structure of R-TiO2/A-TiO2/PBA, demonstrating exceptional photoelectronic properties, significantly enhancing photochromism and secure encryption capabilities. These insights establish a solid foundation for engineering sophisticated complex-ordered nanoarchitectures, advancing sustainable energy and environmental technologies.
Keyword :
homojunction homojunction mixed-valence coordination strategy mixed-valence coordination strategy ordered ternary heterostructure ordered ternary heterostructure photochromism and secure encryption photochromism and secure encryption ultrasmall nanowires ultrasmall nanowires
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GB/T 7714 | Lin, Yalan , Huang, Bingqian , Chen, Yixie et al. Mixed-Valence Coordination Strategy Creating Ordered Ternary Ultrasmall Homo-/Hetero-structures Driven by Lattice Match for Advanced Photochromism and Encryption Applications [J]. | SMALL , 2025 , 21 (16) . |
MLA | Lin, Yalan et al. "Mixed-Valence Coordination Strategy Creating Ordered Ternary Ultrasmall Homo-/Hetero-structures Driven by Lattice Match for Advanced Photochromism and Encryption Applications" . | SMALL 21 . 16 (2025) . |
APA | Lin, Yalan , Huang, Bingqian , Chen, Yixie , Fu, Qingwei , Huang, Haoyang , Zhuang, Zanyong et al. Mixed-Valence Coordination Strategy Creating Ordered Ternary Ultrasmall Homo-/Hetero-structures Driven by Lattice Match for Advanced Photochromism and Encryption Applications . | SMALL , 2025 , 21 (16) . |
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The 3-level features of Latent fingerprints (LFPs) are pivotal in linking suspects with problematic or incomplete fingerprint data, constituting one of the most robust forms of evidence. Aggregation-induced emission (AIE) materials, known for their heightened emissive properties in high aggregation states, provide a robust and powerful approach for developing techniques for 3-level details of LFPs. So far, tremendous efforts have been devoted to solving high background fluorescence interference during the 3-level LFPs visualization process. This review commences with an overview of 3-level features and summarizes the interaction and mechanism of visualizing LFPs involving AIE materials and LFPs secretions. Moreover, it encompasses strategies to enhance the contrast and brightness of 3-level LFPs images. We highlight the mechanism of AIE ' s physicochemical properties and their effects on the visualization of 3-level LFPs. Additionally, we provide insights into potential challenges and opportunities in this emerging field. This paper summarizes the recent development regarding AIE materials for 3-level LFPs visualization, focusing on the visualizing mechanism, engineering strategies, and structure-function relationship. Meanwhile, this review also investigates present challenges and the future directions of AIE materials in this booming research field. image
Keyword :
3-level features 3-level features Aggregation-induced emission Aggregation-induced emission Background interference Background interference Forensic science Forensic science Latent fingerprints detection Latent fingerprints detection
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GB/T 7714 | Zhuang, GuoXin , Wen, YongLin , Lai, XiangHui et al. Recent Progress of Advanced AIE Materials for Visualization of 3-Level Latent Fingerprints [J]. | CHEMPHOTOCHEM , 2024 , 8 (10) . |
MLA | Zhuang, GuoXin et al. "Recent Progress of Advanced AIE Materials for Visualization of 3-Level Latent Fingerprints" . | CHEMPHOTOCHEM 8 . 10 (2024) . |
APA | Zhuang, GuoXin , Wen, YongLin , Lai, XiangHui , Lin, GuoSong , Zhuang, ZanYong , Chen, Fei-Fei et al. Recent Progress of Advanced AIE Materials for Visualization of 3-Level Latent Fingerprints . | CHEMPHOTOCHEM , 2024 , 8 (10) . |
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In modern heterogeneous catalysis, it remains highly challenging to create stable, low-cost, mesoporous 2D photo-/electro-catalysts that carry atomically dispersed active sites. In this work, a general shape-preserving amorphous-to-crystalline transformation (ACT) strategy is developed to dope various transition metal (TM) heteroatoms in ZrO2, which enabled the scalable synthesis of TMs/oxide with a mesoporous 2D structure and rich defects. During the ACT process, the amorphous MZrO2 nanoparticles (M = Fe, Ni, Cu, Co, Mn) are deposited within a confined space created by the NaCl template, and they transform to crystalline 2D ACT-MZrO2 nanosheets in a shape-preserving manner. The interconnected crystalline ACT-MZrO2 nanoparticles thus inherit the same structure as the original MZrO2 precursor. Owing to its rich active sites on the surface and abundant oxygen vacancies (OVs), ACT-CoZrO2 gives superior performance in catalyzing the CO2-to-syngas conversion as demonstrated by experiments and theoretical calculations. The ACT chemistry opens a general route for the scalable synthesis of advanced catalysts with precise microstructure by reconciliating the control of crystalline morphologies and the dispersion of heteroatoms.
Keyword :
amorphous-to-crystalline transformation amorphous-to-crystalline transformation mesoporous 2D materials mesoporous 2D materials oxygen vacancy oxygen vacancy photocatalytic CO2 reduction photocatalytic CO2 reduction scalable synthesis scalable synthesis
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GB/T 7714 | Yan, Jiawei , Luo, Yifei , Zhu, Mengyao et al. General and Scalable Synthesis of Mesoporous 2D MZrO2 (M = Co, Mn, Ni, Cu, Fe) Nanocatalysts by Amorphous-to-Crystalline Transformation [J]. | SMALL , 2024 , 20 (24) . |
MLA | Yan, Jiawei et al. "General and Scalable Synthesis of Mesoporous 2D MZrO2 (M = Co, Mn, Ni, Cu, Fe) Nanocatalysts by Amorphous-to-Crystalline Transformation" . | SMALL 20 . 24 (2024) . |
APA | Yan, Jiawei , Luo, Yifei , Zhu, Mengyao , Yang, Bixia , Shen, Xiaoxin , Wang, Zhiqi et al. General and Scalable Synthesis of Mesoporous 2D MZrO2 (M = Co, Mn, Ni, Cu, Fe) Nanocatalysts by Amorphous-to-Crystalline Transformation . | SMALL , 2024 , 20 (24) . |
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Flexible metal-organic framework (MOF) films are greatly desired for the separation of hazardous molecules and ions from wastewater. The current MOF films are usually horizontally deposited on the substrates, and thus restricted by brittleness, low exposure of surface area, as well as poor separation functions. Here, an organic-inorganic mixed substrate is firstly fabricated by growing hydroxyapatite (HA) nanowire arrays on the cellulose fiber (CF). Subsequently, MIL-100(Fe) nanocrystals are assembled on the surfaces of HA nanowire arrays through a layer-by-layer manner, leading to a unique vertical MOF film. The resulting vertical MOF films show competitive advantages over the horizontal counterparts: (i) they show excellent flexibility and they are tolerant to serious physical damage; (ii) they have multiple separation functions including ion exchange of HA, excellent adsorption of MOFs, and strong electrostatic interaction of CF; and (iii) the agglomeration of MIL-100(Fe) nanocrystals is effectively suppressed. Therefore, the average roughness, specific surface area, and average pore size of films are optimized. As a result, the vertical MOF films show universal separation of positively/ negatively-charged dyes and Pb2+ ion, with high removal rates of > 94 %. More appealing, the mixed pollutants in the complex wastewater can be one-step separated through the vertical MOF films, with high removal rates of > 96 %.
Keyword :
Dyes Dyes Heavy metal ions Heavy metal ions Hydroxyapatite Hydroxyapatite Metal -organic frameworks Metal -organic frameworks Separation Separation
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GB/T 7714 | Gan, Wenxiu , Zheng, Ziyang , Yan, Jiawei et al. Vertical MOF film supported on an organic-inorganic mixed substrate for complex wastewater purification [J]. | APPLIED SURFACE SCIENCE , 2024 , 652 . |
MLA | Gan, Wenxiu et al. "Vertical MOF film supported on an organic-inorganic mixed substrate for complex wastewater purification" . | APPLIED SURFACE SCIENCE 652 (2024) . |
APA | Gan, Wenxiu , Zheng, Ziyang , Yan, Jiawei , He, Xi , Zhuang, Zanyong , Chen, Fei-Fei et al. Vertical MOF film supported on an organic-inorganic mixed substrate for complex wastewater purification . | APPLIED SURFACE SCIENCE , 2024 , 652 . |
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A facile gaseous CO2 mediated solid-to-solid transformation principle is adopted to insert additional CO32- anions into the thin single-crystal nanosheets of Bi2O2CO3, which is built of periodic arrays of intrinsic CO32- anions and (Bi2O2)(2+) layers. The additional CO32- anions create abundant defects. The Bi2O2CO3 nanosheets with rich interlayer CO32- exhibit superior electronic properties and charge transfer kinetics than the pristine single-crystal 2D Bi2O2CO3 and display enhanced catalytic activity in photocatalytic CO2 reduction reaction and the photocatalytic oxidative degradation of organic pollutants. This work thus illustrates interlayer engineering as a flexible means to build layered 2D materials with excellent properties.
Keyword :
2D single crystal 2D single crystal charge transfer charge transfer defect engineering defect engineering interlayer carbonate regulation interlayer carbonate regulation solid-to-solid phase transitions solid-to-solid phase transitions
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GB/T 7714 | Yang, Bixia , Dong, Weilong , Zhu, Chongbing et al. Reinforcing 2D Single-Crystal Bi2O2CO3 with Additional Interlayer Carbonates by CO2-Assisted Solid-to-Solid Phase Transition [J]. | SMALL , 2024 , 20 (35) . |
MLA | Yang, Bixia et al. "Reinforcing 2D Single-Crystal Bi2O2CO3 with Additional Interlayer Carbonates by CO2-Assisted Solid-to-Solid Phase Transition" . | SMALL 20 . 35 (2024) . |
APA | Yang, Bixia , Dong, Weilong , Zhu, Chongbing , Huang, Xinlian , Han, Yunhui , Zheng, Yanting et al. Reinforcing 2D Single-Crystal Bi2O2CO3 with Additional Interlayer Carbonates by CO2-Assisted Solid-to-Solid Phase Transition . | SMALL , 2024 , 20 (35) . |
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Lattice oxygen (O-L) redox chemistry is a key to alleviating the energy and environmental crisis, but it faces challenges in activating the O-L while ensuring structural stability. We disclosed herein that engineering a heterogeneous interface between ultrathin oxide and amorphous carbon can attain the durable O-L redox chemistry without introducing catalytically impure sites. To this end, we proposed a green strategy to grow similar to 3.9 nm-thickness wrinkled delta-MnO2 nanosheets that are rich in defects and are vertically aligned on amorphous carbon spheres. Experiments and calculations reveal that the electrons can easily migrate from the amorphous carbon to MnO2 at the delta-MnO2@C heterointerface. The heterogeneous interfaces can not only regulate the Mn-O bond and create oxygen defects in delta-MnO2 but also introduce lattice oxygen with varying reactivities. Specifically, the delta-MnO2@C structure carries more activated lattice oxygen that contributes to the enhanced activity on catalytic oxidation of bioderived 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA), with a high FDCA formation rate of 1759 mu mol gcat(-1) h(-1) and a high selectivity of 95%. The heterogeneous interface of MnO2@C also brings inert lattice oxygen, so that it manifests high structural stability during the oxidation reactions. This work deepens the fundamental understandings in the engineering of lattice oxygen for durable lattice oxygen redox chemistry and showcases an effective interface technique in creating advanced catalysts for clean sustainable energy.
Keyword :
durable redox chemistry durable redox chemistry Lattice oxygen disproportionation Lattice oxygen disproportionation monodispersed catalyst monodispersed catalyst oxide/carbon heterointerface oxide/carbon heterointerface selective biomass oxidation selective biomass oxidation
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GB/T 7714 | Wang, Yaping , Jiang, Xingpeng , Yang, Bixia et al. Heterointerface of Monodispersed Ultrathin-MnO2@Amorphous Carbon to Attain Durable Lattice Oxygen Redox Chemistry through Creation of Dual Lattice Oxygens [J]. | ACS APPLIED MATERIALS & INTERFACES , 2024 , 16 (43) : 58628-58636 . |
MLA | Wang, Yaping et al. "Heterointerface of Monodispersed Ultrathin-MnO2@Amorphous Carbon to Attain Durable Lattice Oxygen Redox Chemistry through Creation of Dual Lattice Oxygens" . | ACS APPLIED MATERIALS & INTERFACES 16 . 43 (2024) : 58628-58636 . |
APA | Wang, Yaping , Jiang, Xingpeng , Yang, Bixia , Wei, Siyuan , Chen, Yixie , Yan, Jiawei et al. Heterointerface of Monodispersed Ultrathin-MnO2@Amorphous Carbon to Attain Durable Lattice Oxygen Redox Chemistry through Creation of Dual Lattice Oxygens . | ACS APPLIED MATERIALS & INTERFACES , 2024 , 16 (43) , 58628-58636 . |
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In this work, we exploited the synergy between homogeneous and heterogeneous catalysis for the efficient and selective activation of H2O2. The homogeneous catalyst contained a very trace amount of Fe2+ (0.26 ppm), which is lower than the international effluent discharge standard for Fe (0.50 ppm). The heterogeneous catalyst was composed of holey graphitic carbon nitride (g-C3N4) nanosheets carrying highly dispersed single atoms (Mn, Ni, or Cu). Mechanistic studies revealed that the strong interaction between single metal sites and H2O2 forms two adsorption configurations (HOO- and H(O-O)-), which trigger the generation of different reactive oxygen species (ROS). The heterogeneous Mn-C3N4 catalyst provided single Mn-N-3 sites that activated H2O2 to produce O-2 by forming HOO-Mn-N-3, while the adjacent Fe2+ quickly reduced the generated O-2 to O-center dot(2)-, which can efficiently remove organic pollutants and inactivate Escherichia coli under neutral conditions. The single-atom Mn-C3N4, in addition, provided photoactive electrons that drive the efficient cycling of the homogeneous Fe2+/Fe3+ catalyst (which is the rate-determining step) under very trace Fe2+ input. By coupling homogeneous and heterogeneous catalysis, an excellent and advanced oxidation process with potential for large-scale application is reported in this work; the findings also shed light on the theoretical aspects of the efficient and selective activation of H2O2 at the atomic level.
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GB/T 7714 | Yan, Jiawei , Wei, Siyuan , Lin, Yalan et al. Coupling homogeneous and heterogeneous catalysis for the efficient and selective activation of H2O2 [J]. | JOURNAL OF MATERIALS CHEMISTRY A , 2024 , 12 (28) : 17565-17573 . |
MLA | Yan, Jiawei et al. "Coupling homogeneous and heterogeneous catalysis for the efficient and selective activation of H2O2" . | JOURNAL OF MATERIALS CHEMISTRY A 12 . 28 (2024) : 17565-17573 . |
APA | Yan, Jiawei , Wei, Siyuan , Lin, Yalan , Zhu, Yanfei , Zhong, Zhiwu , Zheng, Yanting et al. Coupling homogeneous and heterogeneous catalysis for the efficient and selective activation of H2O2 . | JOURNAL OF MATERIALS CHEMISTRY A , 2024 , 12 (28) , 17565-17573 . |
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