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学者姓名：庄赞勇
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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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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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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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An S-scheme nanoparticle heterojunction of Co3O4-TiO2/C has been designed to enhance CO2 adsorption and accelerate interfacial electron transfer, thereby boosting photocatalytic CO2 reduction. Co2+-loaded MXene nanosheets are used as a single precursor for in situ confined growth of Co3O4-TiO2/C. The in situ confined growth of the nanoparticle heterojunction enables good particle dispersion and a small particle size, which makes the surface and active sites highly exposed and accessible for CO2 molecules. In addition, p-type Co3O4 and n type TiO2 build an S-scheme heterojunction. As a result, the Co3O4-TiO2/C nanoparticle heterojunction exhibits a higher specific surface area, larger CO2 adsorption capacity, and faster charge transfer compared to pure Co3O4 and TiO2/C. The gas generation rate over Co3O4-TiO2/C is as high as 33.21 mmol g-1 h-1, which is 8.34 and 1.69 times higher than that of pure TiO2/C and Co3O4, respectively. 3 h photocatalysis affords a remarkable turnover number of 15.53 that is comparable to state-of-the-art photocatalysts.
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| GB/T 7714 | Liu, Haibing , Chen, Kaihang , Feng, Ya-Nan et al. In Situ Confined Growth of Co3O4-TiO2/C S-Scheme Nanoparticle Heterojunction for Boosted Photocatalytic CO2 Reduction [J]. | JOURNAL OF PHYSICAL CHEMISTRY C , 2023 . |
| MLA | Liu, Haibing et al. "In Situ Confined Growth of Co3O4-TiO2/C S-Scheme Nanoparticle Heterojunction for Boosted Photocatalytic CO2 Reduction" . | JOURNAL OF PHYSICAL CHEMISTRY C (2023) . |
| APA | Liu, Haibing , Chen, Kaihang , Feng, Ya-Nan , Zhuang, Zanyong , Chen, Fei-Fei , Yu, Yan . In Situ Confined Growth of Co3O4-TiO2/C S-Scheme Nanoparticle Heterojunction for Boosted Photocatalytic CO2 Reduction . | JOURNAL OF PHYSICAL CHEMISTRY C , 2023 . |
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Halide perovskites and derivatives have been used as emerging photocatalysts due to their unique optoelectronic and structural diversity. However, compared with the well-explored photophysical processes for light-driven more energetic carriers to trigger redox reactions, catalytic effects on the surface of halide perovskite or their derivatives for chemical transformations between reactive species are seldom addressed, which is equally important for improving the efficiency for halide perovskite-based photocatalysts. Here, we demonstrate that Cs3Bi2Br9 sites in the Cs3Bi2Br9/CdS heterojunction, not only participate in light-driven processes, but also play a vital role for the activation and conversion of key intermediates during C(sp3)-H bond transformation, via a more thermodynamically and kinetically favorable surface reaction pathway. Besides, various aromatic hydrocarbons can be effectively photocatalytic converted to corresponding aldehydes/ketones as major products. This work highlights the importance of surface catalysis mechanism in photocatalysis not only for halide perovskites but also for other semiconductors.
Keyword ：
C-H conversion C-H conversion Heterojunction Heterojunction Perovskite Perovskite Photocatalysis Photocatalysis Surface activation Surface activation
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| GB/T 7714 | Yang, Yalin , Chen, Zheyan , Huang, Hanlin et al. Synergistic surface activation during photocatalysis on perovskite derivative sites in heterojunction [J]. | APPLIED CATALYSIS B-ENVIRONMENTAL , 2023 , 323 . |
| MLA | Yang, Yalin et al. "Synergistic surface activation during photocatalysis on perovskite derivative sites in heterojunction" . | APPLIED CATALYSIS B-ENVIRONMENTAL 323 (2023) . |
| APA | Yang, Yalin , Chen, Zheyan , Huang, Hanlin , Liu, Yuxin , Zou, Junhua , Shen, Shuqi et al. Synergistic surface activation during photocatalysis on perovskite derivative sites in heterojunction . | APPLIED CATALYSIS B-ENVIRONMENTAL , 2023 , 323 . |
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Ordered assembly of anisotropic one-dimensional (1D) and 2D nanomaterials is necessary for preparing delicate heterostructures with close contact to alleviate the energy and environmental crisis. Here, we exploited oriented attachment, a non-classical growth mechanism, as a tool for preparing ordered 1D/2D NiZn layered double hydroxide (Ni-Zn LDH) heterostructures beyond the use of surfactants. Lattice matching between the (101) plane of 1D nanoneedles (NNs) and the (100) plane of 2D nanosheets (NSs) drives the spontaneous ordered assembly of 1D NiZn-LDH NNs on 2D NiZn-LDH NSs. Accordingly, the oxygen-deficient 1D NiZn-LDH capable of CO2 adsorption is, therefore, well dispersed on the 2D platform. The oriented assembly generates strong and intimate interactions between the 1D and 2D units, enabling the efficient transfer of photogenerated electrons from 2D to 1D NiZn-LDH. The oriented 1D/2D NiZn-LDH heterostructure demonstrates superior CO2 photoreduction performance under visible light irradiation, with a CO yield rate of 16,950 mu mol g(-1) h(-1) and a 100% CO selectivity. The findings demonstrate that the growth of anisotropic nanomaterials can be tailored for advanced heterostructure design through oriented attachment alone.
Keyword ：
1D/2D materials 1D/2D materials CO2 photoreduction CO2 photoreduction lattice match lattice match ordered heterostructure ordered heterostructure oriented attachment oriented attachment
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| GB/T 7714 | Zhang, Tingshi , Zhao, Xin , Lin, Mingxiong et al. Surfactant-free synthesis of ordered 1D/2D NiZn-LDH heterostructure through oriented attachment for efficient photocatalytic CO2 reduction with nearly 100% CO selectivity [J]. | SCIENCE CHINA-MATERIALS , 2023 , 66 (6) : 2308-2316 . |
| MLA | Zhang, Tingshi et al. "Surfactant-free synthesis of ordered 1D/2D NiZn-LDH heterostructure through oriented attachment for efficient photocatalytic CO2 reduction with nearly 100% CO selectivity" . | SCIENCE CHINA-MATERIALS 66 . 6 (2023) : 2308-2316 . |
| APA | Zhang, Tingshi , Zhao, Xin , Lin, Mingxiong , Yang, Bixia , Yan, Jiawei , Zhuang, Zanyong et al. Surfactant-free synthesis of ordered 1D/2D NiZn-LDH heterostructure through oriented attachment for efficient photocatalytic CO2 reduction with nearly 100% CO selectivity . | SCIENCE CHINA-MATERIALS , 2023 , 66 (6) , 2308-2316 . |
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An S-scheme nanoparticle heterojunction of Co3O4-TiO2/C has been designed to enhance CO2 adsorption and accelerate interfacial electron transfer, thereby boosting photocatalytic CO2 reduction. Co2+-loaded MXene nanosheets are used as a single precursor for in situ confined growth of Co3O4-TiO2/C. The in situ confined growth of the nanoparticle heterojunction enables good particle dispersion and a small particle size, which makes the surface and active sites highly exposed and accessible for CO2 molecules. In addition, p-type Co3O4 and n type TiO2 build an S-scheme heterojunction. As a result, the Co3O4-TiO2/C nanoparticle heterojunction exhibits a higher specific surface area, larger CO2 adsorption capacity, and faster charge transfer compared to pure Co3O4 and TiO2/C. The gas generation rate over Co3O4-TiO2/C is as high as 33.21 mmol g-1 h-1, which is 8.34 and 1.69 times higher than that of pure TiO2/C and Co3O4, respectively. 3 h photocatalysis affords a remarkable turnover number of 15.53 that is comparable to state-of-the-art photocatalysts.
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| GB/T 7714 | Liu, Haibing , Chen, Kaihang , Feng, Ya-Nan et al. In Situ Confined Growth of Co3O4-TiO2/C S-Scheme Nanoparticle Heterojunction for Boosted Photocatalytic CO2 Reduction [J]. | JOURNAL OF PHYSICAL CHEMISTRY C , 2023 , 127 (11) : 5289-5298 . |
| MLA | Liu, Haibing et al. "In Situ Confined Growth of Co3O4-TiO2/C S-Scheme Nanoparticle Heterojunction for Boosted Photocatalytic CO2 Reduction" . | JOURNAL OF PHYSICAL CHEMISTRY C 127 . 11 (2023) : 5289-5298 . |
| APA | Liu, Haibing , Chen, Kaihang , Feng, Ya-Nan , Zhuang, Zanyong , Chen, Fei-Fei , Yu, Yan . In Situ Confined Growth of Co3O4-TiO2/C S-Scheme Nanoparticle Heterojunction for Boosted Photocatalytic CO2 Reduction . | JOURNAL OF PHYSICAL CHEMISTRY C , 2023 , 127 (11) , 5289-5298 . |
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Preparation of holey, single-crystal, 2D nanomaterials containing in-plane nanosized pores is very appealing for the environment and energy-related applications. Herein, an in situ topological transformation is showcased of 2D layered double hydroxides (LDHs) allows scalable synthesis of holey, single-crystal 2D transition metal oxides (TMOs) nanomesh of ultrathin thickness. As-synthesized 2D Co/NiO-2 nanomesh delivers superior photocatalytic CO2-syngas conversion efficiency (i.e., V-CO of 32460 mu mol h(-1) g(-1) CO and VH2${V_{{{\rm{H}}_2}}}$ of 17840 mu mol h(-1) g(-1) H-2), with V-CO about 7.08 and 2.53 times that of NiO and 2D Co/NiO-1 nanomesh containing larger pore size, respectively. As revealed in high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM), the high performance of Co/NiO-2 nanomesh primarily originates from the edge sites of nanopores, which carry more defect structures (e.g., atomic steps or vacancies) than basal plane for CO2 adsorption, and from its single-crystal structure adept at charge transport. Theoretical calculation shows the topological transformation from 2D hydroxide to holey 2D oxide can be achieved, probably since the trace Co dopant induces a lattice distortion and thus a sharp decrease of the dehydration energy of hydroxide precursor. The findings can advance the design of intriguing holey 2D materials with well-defined geometric and electronic properties.
Keyword ：
CO2 photoreduction CO2 photoreduction defect structures defect structures holey 2D materials holey 2D materials nanosized pores nanosized pores scalable synthesis scalable synthesis
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| GB/T 7714 | Zhang, Tingshi , Zheng, Yanting , Zhao, Xin et al. Scalable Synthesis of Holey Deficient 2D Co/NiO Single-Crystal Na-Nomeshes via Topological Transformation for Efficient Photocatalytic CO2 Reduction [J]. | SMALL , 2023 , 19 (16) . |
| MLA | Zhang, Tingshi et al. "Scalable Synthesis of Holey Deficient 2D Co/NiO Single-Crystal Na-Nomeshes via Topological Transformation for Efficient Photocatalytic CO2 Reduction" . | SMALL 19 . 16 (2023) . |
| APA | Zhang, Tingshi , Zheng, Yanting , Zhao, Xin , Lin, Mingxiong , Yang, Bixia , Yan, Jiawei et al. Scalable Synthesis of Holey Deficient 2D Co/NiO Single-Crystal Na-Nomeshes via Topological Transformation for Efficient Photocatalytic CO2 Reduction . | SMALL , 2023 , 19 (16) . |
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One hurdle in developing transition metal oxide (TMO) catalysts for aerobic oxidation reactions is their need for a low binding energy of the lattice oxygen (O-L) to create active O-L and a high O-L binding energy to maintain structural stability during catalysis. In this work, we prepared amorphous Zr-doped manganese oxide (amor-Zr:MnOx) catalysts carrying dual lattice oxygens that can address such conflicting objectives in catalyst development. In the aerobic oxidation of 5-(hydroxymethyl)furfural (HMF), the amor-Zr0.2MnOx catalyst gave 99% selectivity for 2,5-furandicarboxylic acid (FDCA) and a high FDCA formation rate of 3600 mu mol(FDCA) g(cat)(-1) h(-1) in 1 h. To the best of our knowledge, the aerobic oxidation performance of the amor-Zr0.2MnOx catalyst is superior to those of most Mn-based and related TMO-based catalysts under comparable conditions. Experimental and theoretical studies show that the O-L in amor-Zr: MnOx can be divided into two groups. One group includes the more stable O-L that strengthens the catalyst structure and prevents phase transition, while the other group includes the more reactive O-L that improves catalyst activity through the strong adsorption/activation of O-2 and helps regenerate O-L during catalysis.
Keyword ：
amorphous catalyst amorphous catalyst biomass transformation biomass transformation dual lattice oxygens dual lattice oxygens manganese oxide manganese oxide selective oxidation reaction selective oxidation reaction
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| GB/T 7714 | Wen, Yonglin , He, Lairan , Li, Hu et al. Dual lattice oxygens in amorphous Zr-doped manganese oxide for highly efficient aerobic oxidation of 5-hydroxymethylfurfural to 2,5-furandicarboxylic acid [J]. | SCIENCE CHINA-MATERIALS , 2023 , 66 (5) : 1829-1836 . |
| MLA | Wen, Yonglin et al. "Dual lattice oxygens in amorphous Zr-doped manganese oxide for highly efficient aerobic oxidation of 5-hydroxymethylfurfural to 2,5-furandicarboxylic acid" . | SCIENCE CHINA-MATERIALS 66 . 5 (2023) : 1829-1836 . |
| APA | Wen, Yonglin , He, Lairan , Li, Hu , Han, Yunhui , Zhang, Yiming , Zhuang, Zanyong et al. Dual lattice oxygens in amorphous Zr-doped manganese oxide for highly efficient aerobic oxidation of 5-hydroxymethylfurfural to 2,5-furandicarboxylic acid . | SCIENCE CHINA-MATERIALS , 2023 , 66 (5) , 1829-1836 . |
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