物理化学学报 >> 2021, Vol. 37 >> Issue (6): 2011033.doi: 10.3866/PKU.WHXB202011033
所属专题： 先进光催化剂设计与制备
氧化物钙钛矿的光催化研究进展：CO2还原、水裂解、固氮
王则鉴1,2, 洪佳佳1,2, Ng Sue-Faye3, 刘雯1,2, 黄俊杰1,2, 陈鹏飞1,2,4, Ong Wee-Jun2,3,5,*(
)
- 1 武汉理工大学材料科学与工程学院，武汉 430070
2 武汉理工大学铸材大学生创新创业基地，武汉 430070
3 School of Energy and Chemical Engineering, Xiamen University Malaysia, Selangor Darul Ehsan 43900, Malaysia
4 武汉理工大学，硅酸盐建筑材料国家重点实验室，武汉 430070
5 厦门大学化学化工学院，福建 厦门 361005
-
收稿日期:2020-11-10录用日期:2020-12-08发布日期:2020-12-21 -
通讯作者:Ong Wee-Jun E-mail:weejun.ong@xmu.edu.my; ongweejun@gmail.com -
作者简介:Wee-Jun Ong received his B.Eng. and Ph.D. in chemical engineering from Monash University. He is an Associate Professor in School of Energy and Chemical Engineering at Xiamen University Malaysia. Previously, he was a staff scientist at Agency for Science, Technology and Research (A*STAR), Singapore from 2016 to 2018. In 2019, he was a visiting scientist in Professor Xinliang Feng’s group at Technische Universität Dresden, Germany. In 2019, he was a visiting professor at Lawrence Berkeley National Laboratory, USA. His research interests include the design of nanomaterials for photocatalytic, photoelectrocatalytic, and electrochemical H2O splitting, CO2 reduction, and N2 fixation. He received Global Highly Cited Researcher from Clarivate Analytics for a consecutive 2 years (2019–2020). For more details, refer to https://sites.google.com/site/ wjongresearch/ and https://www.x-mol.com/groups/wee-jun_ong. -
基金资助:武汉理工大学铸材大学生创新创业基地研究基金(S2020001016);厦门大学马来西亚研究基金(XMUMRF/2019-C3/IENG/0013);马来西亚高等教育部基础研究资助项目(FRGS/1/2020/TK0/XMU/02/1)
Recent Progress of Perovskite Oxide in Emerging Photocatalysis Landscape: Water Splitting, CO2 Reduction, and N2 Fixation
Zejian Wang1,2, Jiajia Hong1,2, Sue-Faye Ng3, Wen Liu1,2, Junjie Huang1,2, Pengfei Chen1,2,4, Wee-Jun Ong2,3,5,*()
- 1 School of Materials Science and Engineering, Wuhan University of Technology, Wuhan 430070, China
2 "Zhucai" Center of Innovation and Entrepreneurship, Wuhan University of Technology, Wuhan 430070, China
3 School of Energy and Chemical Engineering, Xiamen University Malaysia, Selangor Darul Ehsan 43900, Malaysia
4 State Key Laboratory of Silicate Materials for Architectures, Wuhan University of Technology, Wuhan 430070, China
5 College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, Fujian Province, China
-
Received:2020-11-10Accepted:2020-12-08Published:2020-12-21 -
Contact:Wee-Jun Ong E-mail:weejun.ong@xmu.edu.my; ongweejun@gmail.com -
About author:Wee-Jun Ong, Email: weejun.ong@xmu.edu.my; ongweejun@gmail.com
-
Supported by:the Research Fund from the "Zhucai" Center of Innovation and Entrepreneurship of Wuhan University of Technology, China(S2020001016);Xiamen University Malaysia Research Fund(XMUMRF/2019-C3/IENG/0013);Ministry of Higher Education (MOHE) Malaysia under the Fundamental Research Grant Scheme (FRGS)(FRGS/1/2020/TK0/XMU/02/1)
摘要：
在寻求可再生能源供应及解决环境问题的迫切需求下，光电、光催化、电催化等领域中多种技术被开发以解决这一迫切问题。其中，光催化技术因其可将清洁太阳能转化为化学燃料的优越能力而备受关注。在层出不穷的光催化材料中，具有阳离子可替代性的钙钛矿氧化物(ABO3)在电子信息、太阳能电池和光催化等领域具有极大的潜力。由于这类材料具有活性高、成本低、稳定性好、结构易调控等独特性能，钙钛矿氧化物光催化剂在水分解、二氧化碳还原转化、固氮等方面取得了广泛的应用。本文综述了光催化的结构与合成方法，重点介绍了光催化的应用，最后展望了光催化的未来发展前景。
MSC2000:
- O643
引用本文
王则鉴, 洪佳佳, Ng Sue-Faye, 刘雯, 黄俊杰, 陈鹏飞, Ong Wee-Jun. 氧化物钙钛矿的光催化研究进展：CO2还原、水裂解、固氮[J]. 物理化学学报, 2021, 37(6): 2011033.
Zejian Wang, Jiajia Hong, Sue-Faye Ng, Wen Liu, Junjie Huang, Pengfei Chen, Wee-Jun Ong. Recent Progress of Perovskite Oxide in Emerging Photocatalysis Landscape: Water Splitting, CO2 Reduction, and N2 Fixation[J]. Acta Phys. -Chim. Sin., 2021, 37(6): 2011033.
Fig 1
(a) Basic principles of photocatalysis on semiconductor 105. Reproduced with permission from American Chemical Society. (b) Mechanisms of photocatalytic overall water splitting 32. Reproduced with permission from American Chemical Society."
Fig 1
Fig 2
(a) Element composition of reported perovskite oxide-based photocatalysts for CO2 reduction 106. Reproduced with permission from Wiley-VCH. (b) The structure of ABO3."
Fig 2
Fig 3
Schematic crystal structures of (a) the monoclinic NaTaO3; (b) the orthorhombic NaTaO3 110. Reproduced with permission from Elsevier. (c) Schematic crystal structures of cubic, orthorhombic and tetragonal KNbO3 109. Reproduced with permission from Royal Society of Chemistry."
Fig 3
Fig 4
(a) Schematic of photoexcitation in a photocatalyst and the redox potential values for the formation of different products at pH = 0 vs. NHE. (b) Band gap and band positions of pristine and doped perovskite materials 13. Reproduced with permission from American Chemical Society."
Fig 4
Fig 5
Schematic for bandgap engineering of semiconductors. The band structure and optical absorption curves of (a) an intrinsic semiconductor, (b) doping-induced intraband energy states, (c) doping-induced band gap narrowing and (d) degenerate doping-induced LSPR 137. Reproduced with permission from Royal Society of Chemistry."
Fig 5
Fig 6
Band structure of various types of heterojunctions in a photocatalytic hybrid composite: (a) Type Ⅱ heterojunction, (b) p-n junction, (c) Schottky junction, (d) Z-scheme heterojunction 11. Reproduced with permission from Elsevier."
Fig 6
Fig 7
(a) Schematic representation of LaFeO3 preparation 152. Reproduced with permission from Elsevier. (b) Schematic process for the preparation of PFN powders 153. Reproduced with permission from Elsevier. (c) Proposed synthesis process of SrFe0.5Ta0.5O3 nanoparticles via the low-temperature solvothermal method 154. Reproduced with permission from Elsevier."
Fig 7
Table 1
Summary of perovskite oxide based materials for photocatalytic CO2 conversion."
| Photocatalyst | Light | Reaction conditions | Cocatalyst (%, w) | Main product(s) | Product evolution | Ref. |
| SrTiO3 | λ > 400 nm | CO2 + H2O | Rh, Au | CO, H2 | 369.2 μmol?g?1?h?1 | |
| 69.4 μmol?g?1?h?1 | ||||||
| NaTaO3 | 300 W UV-enhanced Xe lamp | CO2 + H2O + H2 | Pt (0.5) | CO | 139.1 μmol?g?1?h?1 | |
| NaTaO3 | 300 W UV-enhanced Xe lamp | CO2 + H2O + H2 | Ru (0.5) | CO, CH4 | 51.8 μmol?g?1?h?1 | |
| NaNbO3 | UV (λ < 365 nm) | CO2 : H2O = 7.25 | CO | 11.5 μmol?g?1?h?1 | ||
| KTaO3 | 300 W Xenon arc lamp | CO2 + H2O | Pt (0.5) | H2, CO, O2 | 3780.92 × 10?6 g?1?h?1, 0.00 × 10?6 g?1?h?1, | |
| 2038.80 × 10?6 g?1?h?1 | ||||||
| KTaO3 | 300 W Xenon arc lamp | CO2 + H2O | Ag (0.01) | H2, CO, O2 | 1134.38 × 10?6 g?1?h?1, 152.62 × 10?6 g?1?h?1, | |
| 499.98 × 10?6 g?1?h?1 | ||||||
| CsPbBr3 quantum dot | 300 W Xe lamp | CO2 + H2O | CO, CH4 | 4.3 μmol?g?1?h?1, 1.5 μmol?g?1?h?1 | ||
| BaCeO3 | 300 W Xe lamp | CO2 + H2O | Ag (0.3) | CH4 | 0.55 μmol?g?1?h?1 | |
| LiTaO3 | 200 W Hg-Xe lamp | CO2 + H2 | CO | 0.42 μmol?g?1?h?1 |
Table 1
Table 2
Electrochemical reactions involved in CO2 reduction with water and their corresponding reduction potential E0 106."
| Entry | Equation | Product | E0(V) vs. NHE at pH 7 |
| 1 | CO2 + e? → ?CO2? | Carbonate anion radical | ?1.90 |
| 2 | CO2 + 2H+ + 2e? → HCOOH | Formic acid | ?0.61 |
| 3 | CO2 + 2H+ + 2e? → CO + H2O | Carbon monoxide | ?0.53 |
| 4 | CO2 + 4H+ + 4e? → HCHO + H2O | Formaldehyde | ?0.48 |
| 5 | CO2 + 6H+ + 6e? → CH3OH + H2O | Methanol | ?0.38 |
| 6 | CO2 + 8H+ + 8e? → CH4 + H2O | Methane | ?0.24 |
Table 2
Fig 8
(a) Band structures for a selection of perovskite oxides and oxynitrides and the corresponding redox potentials involved in photocatalytic CO2 reduction 169. Reproduced with permission from American Chemical Society. (b) Mechanism illustration of the photocatalytic CO2 reduction process 191. Reproduced with permission from Elsevier."
Fig 8
Fig 9
(a) The FTIR spectra of gaseous feed, and products of CO2 + CH4 photocatalysis after 4 h visible irradiation on BZ11 (the powders containing BiFeO3 : ZnO with 1 : 1) sample. (b) The possible reaction mechanism of C1 products from CO2 reduction 52. Reproduced with permission from Elsevier."
Fig 9
Fig 10
(a) Band structure scheme for as-prepared NaTaO3-C photocatalyst and samples annealed from 500 ℃ to 700 ℃ 115. Reproduced with permission from Elsevier. (b) Schematic representations of light reflections and refractions in hollow CaTiO3 201. Reproduced with permission from Elsevier."
Fig 10
Fig 11
(a) Ag2CrO4/Ag/BiFeO3@RGO heterojunction showing movement of charge carriers; Photocatalytic CO2 reduction under visible light. (b) Yield of CH4. (c) Yield of CO. The band energy schematic diagram of BiFeO3 and ZnO 203. Reproduced with permission from Elsevier. (d) Before contact, and (e) after making p-n heterojunction along with the mechanism of visible light induced photoreduction of CO2 52. Reproduced with permission from Elsevier."
Fig 11
Fig 12
(a) Low-magnification and (b) high-magnification SEM images of LaCoO3 sample 103. Reproduced with permission from Royal Society of Chemistry."
Fig 12
Fig 13
(a) SEM image of Pt2/3DOM-SrTiO3. (b, c) TEM and HRTEM images of 3DOM SrTiO3 55. Reproduced with permission from Elsevier."
Fig 13
Fig 14
Schematic of photocatalytic CO2 reduction with H2O to CO and CH4 products over Ptn/3DOM-SrTiO3 catalysts 55. Reproduced with permission from Elsevier."
Fig 14
Table 3
Summary of perovskite oxide based materials for photocatalytic water splitting."
| Photocatalyst | Light Source | Reaction conditions | Cocatalyst/% (w) | Activities (μmol?g?1?h?1) | Ref. | |
| H2 Evolution | O2 Evolution | |||||
| SrTiO3 | UV | 1/2.4 vol% methanol | Pt (0.05) | 370 | ||
| SrTiO3 | Vis | 15% diethanolamine aqueous solution +0.5 mmol?L?1 Eosin Y | Pt (0.05) | 90 | ||
| NaTaO3 | λ > 270 nm | Pure water (AgNO3 or CH3OH) | NiO (0.05) | 2180 (16800 in 10 vol% CH3OH) | 1100 (860 in 0.05 mol?L?1 AgNO3) | |
| NaTaO3 (monoclinic) | 400 W high-pressure mercury lamp | Pure water | 2050 | 900 | ||
| NaTaO3 | UV | 5 vol% methanol | 36750 | |||
| NaTaO3 | UV (λ > 200 nm) | Doubly distilled water | NiO (0.4) | 1100 | 500 | |
| NaNbO3(cubic) | λ > 300 nm | 220 mL distilled water + 50 mL CH3OH | Pt (0.5, 1.0, 1.5) | 127.7, 156.1, 97.3 | ||
| NaNbO3 | UV | 5 vol% methanol | 950 | |||
| SrSnO3 (nano) | UV | Distilled water | NiOx (1) | 235.6 | ||
| KNbO3 | UV | 5 vol% methanol | 100 | |||
| KTaO3 | UV | 5 vol% methanol | 1040 | |||
| CaTiO3 | UV | Aqueous methanol solutions (volume ratio 1/20) | NiOx | 670.1 (325.4) | ||
| g-C3N4/SrTa2O6 | 300 W Xenon lamp | Deionized water containing 5% of triethanolamine | Pt | 137000 of g-C3N4 (811700 of SrTa2O6) | ||
| HCa2Nb3O10/Ru complex-CH3 | 300 W Xenon lamp | 100 mL of 10 mmol?L?1 EDTA | Pt | 2400 | ||
| BaZrO3/BaTaO2N | 300 W Xenon lamp | 100 mL of 1.0 mmol?L?1 NaI | Pt | 430 | 950 | |
| Graphene/YInO3 | 300 W Xenon arc lamp | 100 mL solution containing 0.0025 mol Na2S and 0.0025mol Na2SO3 | 400.4 | |||
Table 3
Fig 15
(a) Basic principle of photocatalytic hydrogen and oxygen production via water splitting. (b) Energy band structure and energy level of photocatalytic decomposition of water 241. Reproduced with permission from Elsevier."
Fig 15
Fig 16
(a) Water splitting activity of SrTiO3 photocatalysts. SEM images of SrTiO3 particles: (b) S TO(pristine), (c) STO(flux-Y), and (d) STO(flux-Al) 245. Reproduced with permission from Royal Society of Chemistry."
Fig 16
Fig 17
The morphology engineering strategy for SrTiO3 nanocrystals. (a-c) The morphology of 6-facet SrTiO3 nanocrystals. (d) The structure of the (001) facet of SrTiO3. (e) The schematic description of changing SrTiO3 nanocrystals from 6-facet to 18-facet. (f-h) The morphology of 18-facet SrTiO3 nanocrystals. (ⅰ) The structure of the (001) facet of SrTiO3 246. Reproduced with permission from Royal Society of Chemistry."
Fig 17
Fig 18
(a) H2 (●) and O2 (○) evolution from bulk NiOSrTiO3 (solid line), 30 nm NiOSrTiO3 (dashed line), and 6.5 nm NiOSrTiO3 (dotted line) in 50 mL of water at pH = 7 under full spectrum irradiation (~26.3 mmol?L?1?cm-2 in the UV from 250 to 380 nm) 247. Reproduced with permission from American Chemical Society. (b) Crystal structures of layered perovskites 248. Reproduced with permission from Elsevier. (c) Time course of hydrogen evolution over (●) Rh(0.03)-doped Ca-Nb-O sheets, (■) Rh(0.03)-doped KCa2Nb3O10, and (▲) Rh(1.0 wt%)-loaded Ca-Nb-O sheet. (d) Crystal structure of Rh-doped calcium niobate nanosheet prepared by exfoliation of layered KCa2Nb3-xRhxO10?δ and photocatalytic reaction model in water/methanol system 116. Reproduced with permission from American Chemical Society. (e) Possible charge transfer in the CN/KCTO 2D-2D heterojunction photocatalysts and the corresponding mechanism for their excellent photocatalytic activity 249. Reproduced with permission from Royal Society of Chemistry."
Fig 18
Fig 19
(a) Long-term stability test of LNO-RGO composite for 36 h. (b) Photocatalytic hydrogen production mechanism of LNO-RGO nanoreactor 144. Reproduced with permission from Elsevier."
Fig 19
Table 4
Summary of perovskite oxide based materials for photocatalytic N2 fixation."
| Photocatalyst | Light source | Reaction conditions | Sacrificial agent | NH3 production rate | Ref. |
| CeO2-BiFeO3 | UV-Vis | Deionized water + nitrogen (Acidic medium nitrogen) | none | 117.77 μmol?g?1?h?1 (129.16 μmol?g?1?h?1 (pH = 4)) | |
| TiO2/SrTiO3/g-C3N4 | 300-W Xe lamp | 10-vol% methanol + nitrogen (100 mL?min?1) | ethanol | 2192.0 μmol?L?1?g?1?h?1 | |
| Ag-KNbO3 | 300 W Xe lamp | 5 vol% ethanol | ethanol | 385.0 μmol?L?1?g?1?h?1 | |
| LaCoO3:Er3+/ATP | Visible | Water + nitrogen (2 L?min?1) | ethanol | 71.5 μmol?g?1?h?1 | |
| Bi-Bi2WO6 | Simulated solar light | Water + nitrogen | none | 86.0 μmol?g?1?h?1 | |
| c-PAN-Bi2WO6 | Simulated solar light | Water + nitrogen | none | 160.0 μmol?g?1?h?1 |
Table 4
Fig 20
(a) Schematic of photocatalytic N2 fixation to NH3 on a semiconductor based photocatalyst 293. Reproduced with permission from Elsevier. (b) Generic mechanisms for nitrogen reduction to ammonia on heterogeneous catalysts 294. Reproduced with permission from Elsevier."
Fig 20
Fig 21
(a) Schematic illustration of the formation mechanism of Or-Bi/Bi2WO6 275. Reproduced with permission from Royal Society of Chemistry. (b) Possible mechanisms in Ag/KNbO3 composite under simulated sunlight and visible light 274. Reproduced with permission from American Chemical Society. (c) The photocatalytic mechanism of TiO2/SrTiO3/g-C3N4 heterojunctions under simulated sunlight irradiation. (d) The amount of nitrogen fixation per gram of sample under simulated sunlight irradiation 121. Reproduced with permission from Royal Society of Chemistry. (e) Charge transfer mechanism through the p-n junction in the MCeO2-BiFeO3 composite 273. Reproduced with permission from American Chemical Society. (f) Schematic illustration of the design and preparation of the as-fabricated BP hybrid photocatalyst 276. Reproduced with permission from American Chemical Society."
Fig 21
Fig 22
Schematic of the general mechanism for photocatalytic pollutant degradation 13. Reproduced with permission from American Chemical Society."
Fig 22
Fig 23
Illustration of energy band for pristine BiFeO3 and hydrogenated BiFeO3 with oxygen vacancies 309. Reproduced with permission from Elsevier."
Fig 23
Fig 24
Reaction kinetics for NaNbO3 and reduced NaNbO3 in different temperature 310. Reproduced with permission from Royal Society of Chemistry."
Fig 24
Fig 25
BET surface area plots for (a) g-C3N4, (b) CaTiO3 and (c) CTCN heterojunction. (d) Mechanism of degradation of pollutants under sunlight irradiation using the CTCN heterojunction photocatalyst. (e) Degradation percentage plots of RhB with sunlight irradiation after 120 min of irradiation 24. Reproduced with permission from Beilstein-Institut Zur Forderung der Chemischen Wissenschaften."
Fig 25
Fig 26
Electronic band structure (a) and density of states (b) of barium bismuthate sample 314. Reproduced with permission from Royal Society of Chemistry."
Fig 26
Fig 27
(a) Calculated band structures, total density of states, and partial density of states of constituent elements of Sr2TiO3F2, and Fermi level is marked by dotted orange line; (b) Density contour maps of Sr2TiO3F2 at VBM and CBM 33. Reproduced with permission from Elsevier."
Fig 27
Fig 28
Local structures of optimized configurations for (a) C-doped, (b) Si-doped, (c) N-doped, (d) P-doped, (e) S-doped, (f) Se-doped, (g) F-doped, (h) Cl-doped, (ⅰ) Br-doped and (j) I-doped BaTiO3 with X@O 315. Reproduced with permission from Elsevier."
Fig 28
Fig 29
Total density of states (a) and projected density of states (b) for C-doped, Si-doped, N-doped, P-doped, S-doped and Se-doped systems. The vertical dashed line represents the top of the valence band of the bulk BaTiO3 as the reference level 315. Reproduced with permission from Elsevier."
Fig 29
Fig 30
Schematic representation of the calculated VBM and CBM positions of X-doped BaTiO3 with respect to those of pristine BaTiO3 (a) with X@O and (b) with X@Ti 315. Reproduced with permission from Elsevier."
Fig 30
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