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学者姓名：冯亚南
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Abstract ：
The influence of hydrogen bonding on spectroscopic properties is one of the fundamental issues in the field of luminescent organic-inorganic hybrid metal halides (OIMHs). We design and prepare three OIMHs, namely, crystals 1, 2 and 3, using 2,2 '-bipyridine and ZnCl2 as starting materials. From crystals 1 to 3, the hydrogen bonding environment surrounding the 2,2 '-bipyridinium cations gradually weakens, with both the dihedral angle and the number of hydrogen bonds around them decreasing progressively. Correspondingly, the blue emission belonging to the S1 -> S0 transition of the three crystals gradually increases, with crystal 3 exhibiting the strongest blue light emission and a photo-luminescence quantum yield reaching 34.10%. In crystal 1, the dense hydrogen bonding environment of the 2,2 '-bipyridinium cation results in an obvious energy transfer from S1 to T1. This reduces the population of the S1 state, thereby leading to weaker blue light emission. In crystals 2 and 3, the weaker hydrogen bonding environment and smaller spatial distortion of organic cations weaken or even prevent energy transfer between S1 and T1, thereby enhancing blue light emission. These findings provide new insights for exploring novel luminescent OIMHs and developing more effective means of regulating their luminescence performance. (sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)-(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic) (sic)(OIMHs)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic). (sic)(sic)(sic)2,2 '-(sic)(sic)(sic)(sic)ZnCl2(sic)(sic)(sic), (sic) (sic)(sic)(sic)(sic)(sic)(sic)(sic)OIMH, (sic)(sic)(sic)1,2(sic)3. (sic)(sic)(sic)1(sic)(sic)(sic)3, 2,2 '-(sic)(sic)(sic) (sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic), (sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic) (sic). (sic)(sic)(sic), (sic)(sic)(sic)(sic)(sic)S1 -> S0(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic), (sic)(sic)(sic)(sic)3 (sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic), (sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)34.10%. (sic)(sic)(sic)1(sic), 2,2 '-(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)S1(sic)T1(sic)(sic)(sic)(sic)(sic)(sic)(sic). (sic)(sic) (sic)(sic)S1(sic)(sic)(sic)(sic)(sic), (sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic). (sic)(sic)(sic)(sic)2(sic)3(sic), (sic)(sic)(sic) (sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)S1(sic)T1(sic)(sic)(sic) (sic)(sic)(sic)(sic), (sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic). (sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)OIMHs(sic) (sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic).
Keyword ：
blue emission blue emission hydrogen bonding hydrogen bonding optical materials optical materials organic-inorganic hybrid metal halides organic-inorganic hybrid metal halides photoluminescence photoluminescence
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| GB/T 7714 | Zhang, Qi , Huang, Tianwen , Liu, Zheyuan et al. Hydrogen bonding evolution and efficient blue light emission in a series of Zn-based organic-inorganic hybrid metal halide crystals [J]. | SCIENCE CHINA-MATERIALS , 2025 , 68 (4) : 1004-1011 . |
| MLA | Zhang, Qi et al. "Hydrogen bonding evolution and efficient blue light emission in a series of Zn-based organic-inorganic hybrid metal halide crystals" . | SCIENCE CHINA-MATERIALS 68 . 4 (2025) : 1004-1011 . |
| APA | Zhang, Qi , Huang, Tianwen , Liu, Zheyuan , Feng, Ya-Nan , Yu, Yan , Li, Lingyun . Hydrogen bonding evolution and efficient blue light emission in a series of Zn-based organic-inorganic hybrid metal halide crystals . | SCIENCE CHINA-MATERIALS , 2025 , 68 (4) , 1004-1011 . |
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In this study, divalent calcium cation with large radius and trivalent yttrium cation with small radius were introduced to develop co-stabilized zirconia ceramics with both superior mechanical properties and aging resistance. Through a reverse coprecipitation-hydrothermal method, a series of ultrafine xCaO-yY2O3-ZrO2 (x = 2.0, 3.0, y = 0.5, 1.0, 1.5, 2.0) raw powders with high quality were fabricated for the production of nanostructured ceramics via low-temperature pressurelessly sintering. The sintering process was optimized by investigating the effects of sintering temperature on densification, grain growth and phase evolution. The minimally doped 2.0CaO-0.5Y2O3-ZrO2 ceramic retained pure tetragonal phase at room temperature, achieving a balance of excellent toughness and high aging resistance. The impacts of chemical composition on microstructure, hardness, toughness and aging resistance were examined for these xCaO-yY2O3-ZrO2 (x = 2.0, 3.0, y = 0.5, 1.0, 1.5, 2.0) ceramics. The segregation of calcium and yttrium cations at grain boundaries effectively tailored the microstructure. It was observed that substituting small trivalent yttrium cations for large divalent calcium cations effectively enhanced the aging resistance without sacrificing mechanical properties, due to the strengthened grain boundaries and asymmetrical distribution of cations among grains. This work not only produces low-doped zirconia ceramics with both excellent mechanical properties and aging resistance, but also presents straightforward method for preparation of high-quality raw powders and delicate microstructural engineering during sintering for developing advanced structural ceramics. © 2025 Elsevier Ltd and Techna Group S.r.l.
Keyword ：
Ceramic materials Ceramic materials Grain growth Grain growth High temperature engineering High temperature engineering Low temperature production Low temperature production Microstructural evolution Microstructural evolution Powders Powders Rockwell hardness Rockwell hardness Sintering Sintering Yttria stabilized zirconia Yttria stabilized zirconia Yttrium Yttrium Yttrium metallography Yttrium metallography
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| GB/T 7714 | Feng, Ya-Nan , Wang, Fei-Fan , Xiao, Weiwei et al. Mechanical properties and aging resistance of calcia-yttria co-stabilized zirconia: from powder to ceramic [J]. | Ceramics International , 2025 , 51 (13) : 17368-17378 . |
| MLA | Feng, Ya-Nan et al. "Mechanical properties and aging resistance of calcia-yttria co-stabilized zirconia: from powder to ceramic" . | Ceramics International 51 . 13 (2025) : 17368-17378 . |
| APA | Feng, Ya-Nan , Wang, Fei-Fan , Xiao, Weiwei , Xia, Yan , Wei, Bin , Wang, Shuaihua et al. Mechanical properties and aging resistance of calcia-yttria co-stabilized zirconia: from powder to ceramic . | Ceramics International , 2025 , 51 (13) , 17368-17378 . |
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Developing single-component white-light phosphors remains challenging due to the difficulty in achieving dual emission from mixed-valent activators. Herein, we present a carbon-modulated reduction synthesis (CARS) method to fabricate Eu2+/Eu3+ co-doped La3Si2O8Cl (LSOCl) phosphors without requiring hazardous reducing atmospheres. By modulating carbon content (Eu : C = 1 : 0-2.4), the Eu2+/Eu3+ ratio is effectively controlled, enabling tunable emission from pink to white and yellow under 365 nm UV excitation. The optimized LSOCl:7%Eu (Eu : C = 1 : 1.9) exhibits broadband emission (390-720 nm) with a high color rendering index (Ra = 85.05), cool white light (5489 K, CIE: 0.33, 0.38), and stable performance under varying currents. Additionally, LSOCl:7%Eu (Eu : C = 1 : 1.4) shows excitation-dependent chromaticity shifts: minimal changes under solar-blind UV (250-280 nm) but dramatic variations at 280-350 nm, facilitating rapid detection. A solar-blind UV detector was designed, demonstrating fast response, high resolution (50% CIE shift at 330 nm), and anti-interference capability. The CARS method offers an eco-friendly, scalable route for dual-emission phosphors, showcasing their dual utility in high-quality white LEDs and sensitive UV detection technologies.
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| GB/T 7714 | Chen, Xinhan , Chen, Gaofan , Feng, Ya-Nan et al. Carbon-modulated reduction synthesis of dual-valent Eu-doped La3Si2O8Cl phosphors: single-matrix white LEDs and high-resolution solar-blind UV detection [J]. | JOURNAL OF MATERIALS CHEMISTRY C , 2025 , 13 (21) : 10899-10905 . |
| MLA | Chen, Xinhan et al. "Carbon-modulated reduction synthesis of dual-valent Eu-doped La3Si2O8Cl phosphors: single-matrix white LEDs and high-resolution solar-blind UV detection" . | JOURNAL OF MATERIALS CHEMISTRY C 13 . 21 (2025) : 10899-10905 . |
| APA | Chen, Xinhan , Chen, Gaofan , Feng, Ya-Nan , Zhang, Lizhen , Yu, Yan , Li, Lingyun . Carbon-modulated reduction synthesis of dual-valent Eu-doped La3Si2O8Cl phosphors: single-matrix white LEDs and high-resolution solar-blind UV detection . | JOURNAL OF MATERIALS CHEMISTRY C , 2025 , 13 (21) , 10899-10905 . |
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The strong CO2 adsorption and facile CO desorption are a trade-off issue for CO2-to-CO photoreduction pathways. Synchronous optimization of these two steps remains a substantial hurdle and has been less explored. Herein, an O/N mixed coordinated Co-NTA (NTA: nitrilotriacetic acid), featuring an ultralong nanofiber architecture, is reported for efficient CO2 photoreduction. The mixed coordination can regulate the positions of d-band center of Co sites and also d-p orbital coupling with coordination atoms, which are recognized as main activity descriptors. Consequently, free energies of both steps of CO2 ->*CO2 and *CO -> CO are well optimized, making the CO2-to-CO photoreduction pathways more favorable thermodynamically. By contrast, the classic N-coordinated Co-MeIm (MeIm: 2-methylimidazole) and O-coordinated Co-BDC (BDC: 1,4-benzenedicarboxylic acid) suffer from unfavorable CO2 adsorption and intractable CO desorption, respectively. In addition, achiral NTA molecules can direct the growth of Co-NTA into one-dimensional (1D) nanofibers, while Co-BDC and Co-MeIm possess typical 2D nanosheet and 3D polyhedron architectures. The fast electron transport along the axis directions makes charge-transfer kinetics most efficient over 1D Co-NTA. The thermodynamic and kinetic benefits jointly contribute to the 1.8-fold increase in CO production over 1D Co-NTA.
Keyword ：
d-band center d-band center Metal-organic frameworks Metal-organic frameworks Nanofibers Nanofibers Orbital coupling Orbital coupling
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| GB/T 7714 | Yang, Yong , Jiang, Jianfeng , Feng, Ya-Nan et al. Manipulating d-band center and d-p orbital coupling to mitigate adsorption-desorption trade-off for efficient CO2-to-CO photoreduction over MOF nanofibers [J]. | APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY , 2025 , 379 . |
| MLA | Yang, Yong et al. "Manipulating d-band center and d-p orbital coupling to mitigate adsorption-desorption trade-off for efficient CO2-to-CO photoreduction over MOF nanofibers" . | APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY 379 (2025) . |
| APA | Yang, Yong , Jiang, Jianfeng , Feng, Ya-Nan , Zhuang, Zanyong , Chen, Fei-Fei , Zhang, Dantong et al. Manipulating d-band center and d-p orbital coupling to mitigate adsorption-desorption trade-off for efficient CO2-to-CO photoreduction over MOF nanofibers . | APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY , 2025 , 379 . |
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Fluorescence intensity ratio (FIR)-based optical thermometry, recognized for high reliability and rapid response, has emerged as a promising non-contact temperature sensing technology. This study focuses on enhancing the performance of Er3+/Yb3+ co-doped scheelite-type single crystals (NaY(WO4)2 and NaGd(WO4)2) for wide-range optical temperature sensing. By employing a spontaneous nucleation method, we synthesized single crystals with optimized doping concentrations (1 % Er3+/60 % Yb3+ for NYW and 3 % Er3+/70 % Yb3+ for NGW), achieving intense green upconversion (UC) emissions at 530 nm (2H11/2 -> 4I15/2) and 552 nm (4S3/2 -> 4I15/2). The single crystals exhibited high Yb3+-> Er3+ energy transfer efficiencies of 11.02 % (NYW: 1 % Er3+, 60 % Yb3+) and 20.65 % (NGW: 3 % Er3+, 70 % Yb3+), enabling robust UC luminescence even under harsh conditions (pH = 1/ 13, 72 h) and thermal shocks (800 degrees C, 8 cycles). Temperature-dependent FIR analysis of thermally coupled energy levels (2H11/2 and 4S3/2) revealed linear ln(FIR) vs. 1/T relationships, with maximum relative sensitivities of 1.18 % K-1 (NYW) and 1.12 % K-1 (NGW) in 298-578 K. A prototype sensor utilizing NGW: 3 %Er3+, 70 % Yb3+ single crystal demonstrated practical feasibility across 80-780 K, eliminating fiber-optic requirements due to high UC efficiency. These results highlight scheelite-type single crystals as superior candidates for precision optical thermometry in extreme environments.
Keyword ：
Fluorescence intensity ratio Fluorescence intensity ratio Optical thermometry Optical thermometry Scheelite-type single crystals Scheelite-type single crystals Temperature sensors Temperature sensors Upconversion emission Upconversion emission
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| GB/T 7714 | Wu, Weiqing , Xu, Yurong , Lin, Xinyi et al. Ultra-stable Er3+/Yb3+Co-doped scheelite single crystals for wide-range fiber-free optical thermometry [J]. | JOURNAL OF LUMINESCENCE , 2025 , 283 . |
| MLA | Wu, Weiqing et al. "Ultra-stable Er3+/Yb3+Co-doped scheelite single crystals for wide-range fiber-free optical thermometry" . | JOURNAL OF LUMINESCENCE 283 (2025) . |
| APA | Wu, Weiqing , Xu, Yurong , Lin, Xinyi , Huang, Fazheng , Feng, Ya-Nan , Zhang, Lizhen et al. Ultra-stable Er3+/Yb3+Co-doped scheelite single crystals for wide-range fiber-free optical thermometry . | JOURNAL OF LUMINESCENCE , 2025 , 283 . |
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As a class of emerging photoluminescent materials, hybrid halide crystals have drawn research attention for their potential application in the fields of light-emitting, security, and waveguide. Nevertheless, hybrid halide crystals containing antimony with long-term stability and tunable light emission are still increasingly in demand. In this work, serial new hybrid halide crystals (BZA)(2)ZnCl42H(2)O:xSb(3+) (x = 0-0.2, x represents the reaction ratio) and (BZA)(2)SbCl5 are synthesized (BZA = 2,4-diamino-6-phenyl-1,3,5-triazine). In (BZA)(2)ZnCl42H(2)O:xSb(3+) crystals, Sb3+ cations replace partial Zn2+ cations to form [SbCl4](-) tetrahedron. Red light emission caused by the substitution of Sb3+ for Zn2+ enhances as the doping rate increases, resulting in the tunable emission from light blue to pink and finally to dark red. There are two kinds of Sb3+ in (BZA)(2)SbCl5 crystal. Sb(1) has a sixfold coordination with Cl to form a [Sb(1)Cl-5]infinity 1D zigzag chain. Sb(2) atom adopts a fivefold coordination with Cl and is separated from each other by BZA(+) cations. (BZA)(2)SbCl5 crystal shows bright orange-yellow light emission with a photoluminescence quantum yield of 45%. Moreover, the organic-inorganic hybrid metal halide crystals containing antimony have excellent long-term stability, with phase and luminescence keeping nearly unchanged after more than six months in ambient air.
Keyword ：
hybrid halide crystals hybrid halide crystals Sb3+ Sb3+ stability stability tunable light emission tunable light emission
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| GB/T 7714 | Zhang, Yaqing , Jiang, Yan , Zhang, Qi et al. Antimony Doped Hybrid Zinc Halide Crystals with Tunable Light Emission and Long-Term Stability [J]. | ADVANCED OPTICAL MATERIALS , 2024 , 12 (12) . |
| MLA | Zhang, Yaqing et al. "Antimony Doped Hybrid Zinc Halide Crystals with Tunable Light Emission and Long-Term Stability" . | ADVANCED OPTICAL MATERIALS 12 . 12 (2024) . |
| APA | Zhang, Yaqing , Jiang, Yan , Zhang, Qi , Liu, Qingyi , Guo, Weiping , Zhang, Wei et al. Antimony Doped Hybrid Zinc Halide Crystals with Tunable Light Emission and Long-Term Stability . | ADVANCED OPTICAL MATERIALS , 2024 , 12 (12) . |
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As an important interaction among organic cations containing aromatic rings, the pi-pi stacking interaction is a crucial factor determining the crystal structure of organic-inorganic hybrid metal halides (OIMHs). However, the relationship between pi-pi interaction and optical properties of luminescent OIMHs is yet to be studied. (C10H10N2)Cd1-xZnxCl4 (23-Cd1-xZnxCl4) crystals with 0D structures are synthesized by using optically active 2,3 '-bipyridine as the organic ligand. When x <= 0.2, there is no pi-pi interaction among 2,3 '-bipyridinium cations in 23-Cd1-xZnxCl4 crystals. When x > 0.2, pi-pi interaction among organic cations occurs and enhances as the Zn2+ content increases. The tailoring of the pi-pi interaction endows 23-Cd1-xZnxCl4 with tunable light emitting properties, resulting in a broad band emission involving blue and orange species. The blue emission dominates when there is no pi-pi interaction, while the orange emission enhances and finally becomes dominant as the strength of pi-pi interaction increases. The pi-pi interaction promotes the energy transfer from the higher energy valley to the lower one of the S-1 state of the organic cation, resulting in the enhancement of orange emission. Notably, the 23-ZnCl crystal exhibits a photo-luminescence quantum yield (PLQY) of 32%. This is the highest reported value to date among the Zn-based OIMHs, which have optical emission originating from the organic component. The mechanism of pi-pi stacking induced tunable light emission revealed in our work provides new guidance for the design of luminescent OIMHs.
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| GB/T 7714 | Zhang, Qi , Lin, Xinyi , Guo, Shanji et al. Tailoring the π-π stacking interaction among organic cations in hybrid metal halide crystals towards tunable light emission [J]. | JOURNAL OF MATERIALS CHEMISTRY C , 2024 , 12 (19) : 7053-7061 . |
| MLA | Zhang, Qi et al. "Tailoring the π-π stacking interaction among organic cations in hybrid metal halide crystals towards tunable light emission" . | JOURNAL OF MATERIALS CHEMISTRY C 12 . 19 (2024) : 7053-7061 . |
| APA | Zhang, Qi , Lin, Xinyi , Guo, Shanji , Zhang, Yaqing , Jiang, Yan , Zhang, Wei et al. Tailoring the π-π stacking interaction among organic cations in hybrid metal halide crystals towards tunable light emission . | JOURNAL OF MATERIALS CHEMISTRY C , 2024 , 12 (19) , 7053-7061 . |
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Beyond traditional paper, multifunctional nanopaper has received much attention in recent years. Currently, many nanomaterials have been successfully used as building units of nanopaper. However, it remains a great challenge to prepare flexible and freestanding metal-organic framework (MOF) nanopaper owing to the low aspect ratio and brittleness of MOF nanocrystals. Herein, this work develops a flexible and free-standing MOF nanopaper with MOF nanowires as building units. The manganese-based MOF (Mn-MOF) nanowires with lengths up to 100 mu m are synthesized by a facile solvothermal method. Through a paper-making technique, the Mn-MOF nanowires interweave with each other to form a three-dimensional architecture, thus creating a flexible and free-standing Mn-MOF nanowire paper. Furthermore, the surface properties can be engineered to obtain high hydrophobicity by modifying polydimethylsiloxane (PDMS) on the surfaces of the Mn-MOF nanowire paper. The water contact angle reaches 130 degrees. As a proof of concept, this work presents two potential applications of the Mn-MOF/PDMS nanowire paper: (i) The as-prepared Mn-MOF/PDMS nanowire paper is compatible with a commercial printer. The as-printed colorful patterns are of high quality, and (ii) benefiting from the highly hydrophobic surfaces, the Mn-MOF/PDMS nanowire paper is able to efficiently separate oil from water.
Keyword ：
flexible flexible free-standing free-standing metal-organic frameworks metal-organic frameworks nanopaper nanopaper nanowires nanowires
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| GB/T 7714 | Yang, Yong , Yang, Zhe , Zhuang, Guoxin et al. Flexible and Free-Standing Metal-Organic Framework Nanowire Paper [J]. | ACS APPLIED MATERIALS & INTERFACES , 2024 , 16 (23) : 30306-30313 . |
| MLA | Yang, Yong et al. "Flexible and Free-Standing Metal-Organic Framework Nanowire Paper" . | ACS APPLIED MATERIALS & INTERFACES 16 . 23 (2024) : 30306-30313 . |
| APA | Yang, Yong , Yang, Zhe , Zhuang, Guoxin , Feng, Ya-Nan , Chen, Fei-Fei , Yu, Yan . Flexible and Free-Standing Metal-Organic Framework Nanowire Paper . | ACS APPLIED MATERIALS & INTERFACES , 2024 , 16 (23) , 30306-30313 . |
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Two-dimension nanosheets are ideal photocatalysts for CO2 reduction due to their high exposure of active sites and short charge transfer pathway. However, 2D photocatalysts have a tendency to agglomeration, thus compromising the performance of photocatalytic CO2 reduction. Trees, one of the most important plants for photosynthesis, have a unique "leaf-on-branch" structure. This unique two-dimension/one-dimension (2D/1D) configuration maximizes the adsorption of CO2 molecules and light harvesting. Herein, a tree-inspired semiconductor-on-ceramic 2D/1D heterostructure for efficient photocatalytic CO2 reduction is reported. The cobalt silicate (CoSi) nanosheets (similar to 0.68 nm) are in situ grown on the surfaces of hydroxyapatite (HAP) nanowires, creating a well-defined 2D/1D hierarchical structure. The vertical alignment of ultrathin CoSi nanosheets on the HAP nanowires effectively suppresses their agglomeration, leading to a large BET surface area (106.45 m(2)/g) and excellent CO2 adsorption (8.00 cm(3) g(-1)). The results of photoelectrochemical characterization demonstrate that the 2D/1D hierarchical structure is powerful to expedite charge transfer. As a result, the gas generation rate of CO is as high as 28780 mu mol g(-1) h(-1) over the CoSi-on-HAP 2D/1D heterostructure. In addition, the electron transfer mechanism and reaction pathways of CO2 reduction are revealed by in situ irradiated XPS and in situ DRIFT spectra.
Keyword ：
CO2 reduction CO2 reduction Heterostructure Heterostructure Hydroxyapatite nanowires Hydroxyapatite nanowires Photocatalysis Photocatalysis Silicate nanosheets Silicate nanosheets
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| GB/T 7714 | Hu, Yingzi , Zhu, Yan , He, Xi et al. Tree-inspired semiconductor-on-ceramic 2D/1D heterostructure for efficient CO2 photoreduction [J]. | APPLIED SURFACE SCIENCE , 2024 , 672 . |
| MLA | Hu, Yingzi et al. "Tree-inspired semiconductor-on-ceramic 2D/1D heterostructure for efficient CO2 photoreduction" . | APPLIED SURFACE SCIENCE 672 (2024) . |
| APA | Hu, Yingzi , Zhu, Yan , He, Xi , Feng, Ya-Nan , Chen, Fei-Fei , Yu, Yan . Tree-inspired semiconductor-on-ceramic 2D/1D heterostructure for efficient CO2 photoreduction . | APPLIED SURFACE SCIENCE , 2024 , 672 . |
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Developing efficient and robust artificial hydrogenases with sophisticated structure as catalysts is potential for practical solar hydrogen application, withstanding challenges proposed by oxygen generated in situ by water splitting. Based on Pearson's hard/soft acid/base (HSAB) theory and compartmental ligand strategy, we prepared a 3D heterometallic MOF, [Ni3Pr2(6-mna)6(H2O)4]center dot(H2O)5 (1) (6-mna = 6-mercaptonicotinate divalent anion), with alternately arranged redox-active NiS cluster-based nodes and redox-inactive PrO cluster-based nodes to mimic simultaneously both the active center and the surrounding polypeptide microenvironment in natural hydrogenase. Despite numerous negative effects caused by oxygen, with the sophisticated structure, 1 achieved both enhanced stability and efficient hydrogen producing activity of 40.3 mmol/g in air atmosphere. The influence of oxygen on photocatalytic hydrogen production was investigated by contrasting mechanisms of both photo-induced electron transferring step and chemical catalyzing step under aerobic and anerobic conditions. The reductive mechanism is promoted under anerobic conditions, whereas oxidative mechanism is favored in aerobic conditions due to the suppressed production of radical intermediate Fl3-center dot in the presence of oxygen, as evidenced by in-situ electron spin resonance spectroscopy and in-situ ultraviolet-visible absorption spectrum. This paper presents a simple method for MOFs to closely simulate both the active center and surrounding protein of biological enzymes, and offers a new pathway for developing stable and efficient catalyst for solar hydrogen production.
Keyword ：
Aerobic solar hydrogen production Aerobic solar hydrogen production Artificial hydrogenase Artificial hydrogenase Heterometallic MOF Heterometallic MOF
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| GB/T 7714 | Feng, Ya-Nan , Xia, Yan , Yu, Shu-Wen et al. Mimicking the active site and microenvironment of hydrogenase in a heterometallic MOF with enhancing stability and high efficiency for aerobic solar hydrogen production [J]. | JOURNAL OF ALLOYS AND COMPOUNDS , 2024 , 1010 . |
| MLA | Feng, Ya-Nan et al. "Mimicking the active site and microenvironment of hydrogenase in a heterometallic MOF with enhancing stability and high efficiency for aerobic solar hydrogen production" . | JOURNAL OF ALLOYS AND COMPOUNDS 1010 (2024) . |
| APA | Feng, Ya-Nan , Xia, Yan , Yu, Shu-Wen , Wei, Zhi-Yan , Li, Lingyun , Chen, Fei-Fei et al. Mimicking the active site and microenvironment of hydrogenase in a heterometallic MOF with enhancing stability and high efficiency for aerobic solar hydrogen production . | JOURNAL OF ALLOYS AND COMPOUNDS , 2024 , 1010 . |
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