铜基双金属硫氧、硫硒化物的合成及氧化还原反应｜國立臺灣科技大學博碩士論文系統

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研究生：	陳孝雲 Xiao-Yun Chen
論文名稱：	铜基双金属硫氧、硫硒化物的合成及氧化还原反应 Synthesis of Cu-Based Bimetal Oxysulfide and Seleno-Sulfide Catalysts for Redox Reactions
指導教授：	郭東昊 Dong-Hau Kuo
口試委員:	郭東昊 Dong-Hau Kuo 薛人愷 Ren-Kae Shiue 魏茂國 Mao-Kuo Wei 何清華 Ching-Hwa Ho 邱智瑋 Chih-Wei Chiu
學位類別：	博士 Doctor
系所名稱：	工程學院 - 材料科學與工程系 Department of Materials Science and Engineering
論文出版年：	2017
畢業學年度：	105
語文別：	英文
論文頁數：	296
中文關鍵詞：	双金属硫氧化物、双金属硫硒化物、固溶体催化剂、氧化还原反应、二氧化碳还原、产氢、暗室反应、阴离子空位、机理
外文關鍵詞：	Bimetal oxysulfide catalyst, bimetal seleno-sulfide catalyst, solid-solution catalyst, redox reactions, CO2 conversion, hydrogen production, darkness reaction, anion vacancy, mechanism
相關次數：	點閱：305 下載：0
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見英文部分

Since Fujishima and Honda in 1972 discovered the photoinduced water splitting on TiO2 electrodes, semiconductor-based photocatalysis has been on application for the photodegradation of organic pollutants, photoreduction heavy metal, photocatalytic generation hydrogen, photoreduction CO2 to production methanol, ethanol and other organics, and photocatalytic sterilization. But these application almost need light (ultraviolet light, visible light, or sun light) excitation, so it only can be used in the daytime-outdoor-sunshine reached area or under the artificial light that generated by the electric-driven lamp. However, the light does not reach to all the application area and the use of electric efficiency of electric-to-light-to-electric is less than 10%. Most of electricity is released into the environment through heat, thus the application of photocatalyst has its constraint. To overcome the limitation, the exploration of catalyst for the organic degradation reaction without light has become one of the core challenges in catalysis and pollution control.
This work we report a novel Cu-based bimetal nanoflower oxysulfide and nanosheet seleno-sulfide catalysts by a feasible method for Cr(VI) reduction, organic degradation (MB), hydrogen generation, and CO2 reduction in the normal environmental conditions. Their structures were characterized by field-emission scanning electron microscope (FE-SEM), high resolution transmission electron microscope (HR-TEM), X-ray diffractometry (XRD), Fourier transform infrared spectroscopy (FTIR), ultraviolet–visible diffuse reflectance spectra (UV-Vis DRS), X-ray photoelectron spectroscopy (XPS), photoluminescence emission spectrum (PL), and N2 adsorption-desorption experiments. Accordance to the structures characterization and performances analysis, the reaction kinetic mechanism was proposed. There are five parts in this thesis including CuInOS catalyst for Cr(VI) reduction, CuNiOS for MB redox reactions, CuCoOS for H2 generation, CuMnOS for CO2 conversion, and CuNiSeS for methylene blue (MB) degradation.

Table of contents
Abstract    I
Acknowledgements    IV
Table of contents    V
List of Figures    XI
List of Tables    XXVII
Chapter 1    Introduction    1
1    Background of the study    1
2    Wastewater treatment    2
3    Hydrogen production    4
4    CO2 conversion and utilization    6
5    Research objectives    7
Chapter 2    Literature review and basic theory    9
1    Sulfide-based catalysts    9
1.1    Three-dimensional CuS hierarchical architecture photocatalyst    9
1.2    Nanoflake CuS catalyst    11
1.3    Nanoflower CuS catalyst    12
1.4    Hierarchical wool ball-like CuS microflower catalyst    13
1.5    Concave polyhedral superstructure CuS catalyst    15
1.6    CuxSy catalyst    17
1.7    Hollow nanosphere CuS catalyst    18
1.8    Sphere-like CuS catalyst    19
1.9    Nanodisk Cu2-xS catalyst    21
1.10    Nanorods and shuttle-like bundles CuS catalyst    23
1.11    TiO2 layer coated-CdS spheres core−shell catalyst    24
1.12    Cu2S-incorporated ZnS catalyst    26
1.13    Nanorods Sb2S3 catalyst    27
1.14    CdS–Titanate nanodisk multicomponent catalyst    28
1.15    Core−shell nanowire ZnO/ZnS/CdS/CuInS2 catalyst    30
1.16    Pt-tipped CdS nanorod/CdSe nanoheterostructured catalyst    31
1.17    CdS−cluster-decorated graphene nanosheets catalyst    32
1.18    CdS-AgGaS2 diodes catalyst    33
2    Selenide based catalysts    34
2.1    Nanoflakes stacked Cu2-xSe catalyst for solar cell application    34
2.2    Fernwort-like CuSe catalyst for MG and RhB degradation    36
2.3    Cu2Se nanoparticles catalysts    38
2.4    Cu2-xSe nanocrystals catalyst    40
2.5    Cu2-xSe nanoparticles catalyst    41
2.6    CuSe nanocrystals for photothermal therapy    43
2.7    MoSe2 catalyst for Cr(VI) redction    43
2.8    Hollow CdSe for degradation of tetracycline hydrochloride    45
2.9    SnSe nanosheets catalyst    46
2.10    Ni3Se2 catalyst for oxygen evolution reaction    47
2.11    Flower-like CuSe-ZnSe for MO and MB degradation    49
2.12    ZnO/ZnSe and ZnO/CuSe heterostructures    50
3    Solid solution based catalysts    52
3.1    Nanowire Zn(O,S) catalyst for generation H2    52
3.2    Zn(O,S) nanoparticle catalyst for generation H2    54
3.3    In2(O,S)3 nanosheets catalyst for Cr(VI) reduction and generation H2    55
3.4    Band gap modification of ZnO and ZnS through solid solution formation    56
3.5    Tunable CuSySe1-y nanomaterials    57
3.6    Strong valence-band offset bowing of ZnO1-xSx    58
3.7    Star-shaped Cu2-xSySe1-y materials    59
3.8    Ternary CuSxSe1-x nanoplates materials    60
3.9    Hexagonal Cu2-xSySe1-y nanoplates materials    62
3.10    Cu2-xSeyS1-y and Cu2-xTeyS1-y photocatalyst    63
3.11    CuIn(S1-xSex)2 photocatalyst    65
3.12    BiCu1-xOS oxysulfide photocatalyst    66
3.13    LaCuOS oxysulfide photocatalyst    68
3.14    (LaO)CuS oxysulfide photocatalyst    68
3.15    La3CuO2S3 oxysulfide photocatalyst    70
3.16    CoOxSy oxysulfide photocatalyst    71
3.17    MoOS2 oxysulfide photocatalyst    72
3.18    (CoNi)OxSy oxysulfide photocatalyst    72
3.19    LiNiSyO2-y oxysulfide photocatalyst    73
3.20    In4Sn16O10S34 oxysulfide photocatalyst    74
3.21    Fe@ZnO0.6S0.4 photocatalytic inactivation of Escherichia coli    76
3.22    (Ga1-xZnx)(N1-xOx) solid solution photocatalyst    76
3.23    CaZnOS oxysulfide photocatalyst    77
3.24    Zn1-xCuxO1-ySy) alloy thin films    79
4    Dye degradation catalyst in the dark    80
4.1    Ag–In–Ni–S nanocomposites catalyst for degradation dye in the dark    80
4.2    CuS catalyst for degradation dye with H2O2 imposing in the dark    81
4.3    MoS2 for degradation dyes with ultrasonic wave imposing in the dark    83
4.4    Nickel sulphide nanocomposites catalyst for degradation dyes in the dark    86
4.5    Hybrid CuxO/TiO2 catalyst for VOCs degradation in indoor    88
4.6    CeGeO4 catalyst for degradation dyes in the dark    90
4.7    Ce(IO3)4 and CeGeO4 catalyst for degradation dyes in the dark    91
5    Generation H2 photocatalyst    92
5.1    AgPd-Hs/G catalyst for hydrogen generation    92
5.2    TiO2-Pt nano-wire photocatalyst    94
5.3    Au/Cu2ZnSnS4 core/shell NPs for hydrogen photocatlytic production    95
5.4    Pt/Al2O3 for hydrogen generation    96
5.5    CuZnGaOx catalyst generation hydrogen    97
5.6    ZnO/Pt/Cd1-xZnxS and ZnO/Pt/CdS1-xSex heterostructured photocatalyst    98
5.7    MoS2 nanosheet-coated TiO2 for photocatalytic hydrogen production    100
5.8    (AgIn)xZn2(1-x)S2/Pt photocatalyst    101
5.9    MoS2/ZnIn2S4 nanocomposites for photocatalytic hydrogen generation    102
5.10    Novel stannite-type complex sulfide photocatalyst    103
5.11    AgInZn7S9 photocatalyst    105
6    CO2 Conversion    106
6.1    Bi2S3/CdS reduction CO2 to methanol    106
6.2    Cu/TiO2 catalysts reduction CO2 to methanol    107
6.3    NixGay catalysts reduction CO2 to methanol    108
6.4    Cu/ZnO catalysts reduction CO2 to methanol    108
6.5    AlGaN/GaN conversion CO2 to HCOOH    109
6.6    Cu/ZnO-based catalysts reduction CO2 to methanol    110
6.7    Co-porphyrin/carbon nitride hybrids for CO2 reduction    110
6.8    Cobalt catalysts conversion CO2 to hydrocarbons    112
6.9    Defect-rich CeO2 nanorods catalyst for CO2 conversion    112
6.10    Ruthenium catalyst for conversion CO2 to methanol    114
6.11    CuO/ZnO/Al2O3 catalysts reduction CO2 to CH3OH    114
6.12    Core–shell structure CuxZn1-xOy catalyst for reduction CO2    115
6.13    Zinc-rich copper Cu-ZnOAl2O3 catalyst for methanol synthesis    116
6.14    Na–Fe3O4/HZSM-5 catalyst directly converting CO2 into gasoline fuel    117
Chapter 3    Materials and methods    119
1    Materials    119
1.1    Chemicals    119
1.2    Instruments    120
2    Sythesis of catalysts    121
2.1    Synthesis of CuMOS    121
2.2    Sythesis of CuSeS    121
2.3    Sythesis of CuMSeS    122
3    Performance evaluation    122
3.1    Cr(VI) reduction measurements    122
3.2    MB degradation measurements    123
3.3    Catalytic hydrogen generation    123
3.4    CO2 conversion to fuel measurements    124
3.5    Electrochemical measurements    124
4    Characterization of catalysts    125
4.1    X-ray diffractometry (XRD)    125
4.2    X-ray photoelectron spectroscopy (XPS)    126
4.3    Field emission scanning electron microscopy (FE-SEM)    127
4.4    High resolution transmission electron microscopy (HR-TEM)    127
4.5    UV-Vis Diffuse reflectance spectroscopy (UV-Vis DRS)    128
4.6    Photoluminescence spectroscopy (PL)    129
4.7    Fourier transform infrared spectroscopy (FTIR)    129
4.8    Adsorption/desorption isotherm (BET)    130
Chapter 4    Results and Discussion    131
1    Nanoflower bimetal CuInOS oxysulfide catalyst for the reduction of Cr(VI) in the dark       131
1.1    Introduction    131
1.2    Experimental methods    132
1.3    Results and discussion    134
1.4    Summary    153
2    The effect of the Cu+/Cu2+ ratio on the redox reactions by nanoflower CuNiOS catalysts in the dark    155
2.1    Introduction    155
2.2    Experimental    156
2.3    Results and discussion    158
2.4    Summary    176
3    Nonthermal dehydrogenation of liquid carrier for the hydrogen generation by inorganic catalysts at normal temperature and pressure, even in dark    178
3.1    Introduction    178
3.2    Experimental    179
3.3    Results and discussion    180
3.4    Summary    194
4    CuMnOS nanoflowers with different Cu+/Cu2+ ratios for the CO2-to-CH3OH and the CH3OH-to-H2 redox reactions    195
4.1    Introduction    195
4.2    Experimental    196
4.3    Results    198
4.4    Discussion    210
4.5    Summary    216
5    A novel CuNiSeS bimetal seleno-sulfide catalyst for methylene blue degradation in the dark    218
5.1    Introduction    218
5.2    Experimental    219
5.3    Results and discussion    220
5.4    Summary    233
Chapter 5    Conclutions    235
References    237
Publications and Patents    262


                                

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全文公開日期 2022/06/06 (校內網路)
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