July 11, /07/11 Advanced Course in Photocatalytic Reaction Chemistry 1
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1 July 11, /07/11 Advanced Course in Photocatalytic Reaction Chemistry 1
2 Advanced Course in Photocatalytic Reaction Chemistry understanding chemistry by understanding photocatalysis understanding photocatalysis by understanding chemistry Division of Environmental Material Science, Graduate School of Environmental Science The first semester of Fiscal :45 10:15, Thursday at Lecture Room D103 Bunsho Ohtani, Ewa Kowalska and Mai Takase Catalysis Research Center, Hokkaido University, Sapporo , Japan (dial-in)/ (facsimile) /07/11 Advanced Course in Photocatalytic Reaction Chemistry 2
3 objectives/goal/keywords << objectives >> Understanding the mechanism of decomposition of pollutants, methods of photocatalysts preparation, design of practical photocatalytic reaction systems, and strategy for enhancement of photocatalytic activity. << goal >> To understand principle of photocatalytic reaction from the standpoint of chemistry and strategy for practical applications. To obtain scientific method for research on functional solid materials. << keywords >> Photocatalyst, Photoinduced oxidative decomposition, Superhydrophilicity, Excited electron-positive hole, Structure-activity correlation, Higher photocatalytic activity, Visible-light response 2013/07/11 Advanced Course in Photocatalytic Reaction Chemistry 3
4 schedule (1) April 11 introduction of photocatalysis (2) April 18 interaction between substances and light (3) April 25 electronic structure and photoabsorption (4) May 2 thermodynamics: electron and positive hole (5) May 9 adsorption (6) May 16 (Professor Ewa Kowalska) (7) May 23 kinetic analysis of photocatalysis (8) May 30 steady-state approximation (9) June 6 kinetics and photocatalytic activity (10) June 13 kinetic analysis (11) June 20 action spectrum analysis (1) (12) June 27 (Professor Mai Takase) (13) July 4 action spectrum analysis (2) (14) July 11 crystal structure of titania (15) July 18 design and development of photocatalysts July 25 deadline for submission of special report 2013/07/11 Advanced Course in Photocatalytic Reaction Chemistry 4
5 special report special report for extra score (20 point) report on critical review on "photocatalysis" in Wikipedia, pointing out errors, misunderstanding and speculations 光触媒 Japanese or English A4 size 2 pages submission by attachment a PDF file is more preferable than a Word file title: pc xxxxxxxx file name: pc xxxxxxxx.pdf (or.docx or.dox) deadline of submission: July 25, : /07/11 Advanced Course in Photocatalytic Reaction Chemistry 5
6 comments on this lecture Please send in Japanese or English within 48 hours to: subject: pc2013mmdd-xxxxxxxx body: (full name) (nickname) (comments and/or questions on today's lecture) 2013/07/11 Advanced Course in Photocatalytic Reaction Chemistry 6
7 action spectrum analysis action spectrum analysis 2013/07/11 Advanced Course in Photocatalytic Reaction Chemistry 7
8 unit cell of crystal unit of repetition: connected to all directions Atoms (ions) are shown in a dot at their center Apexes are occupied by atoms (ions), which are shared by unit cells. x-y-z (a-b-c) is set as a right hand. c β α γ b a 2013/07/11 Advanced Course in Photocatalytic Reaction Chemistry 8
9 two-dimensional unit cells /07/11 Advanced Course in Photocatalytic Reaction Chemistry 9
10 two-dimensional unit cells /07/11 Advanced Course in Photocatalytic Reaction Chemistry 10
11 a game: a practice for making a quiz first: circle/second: cross Both don't like to be beaten. Q Which, first or second, will win? A At seventh, the first won. Why? 2013/07/11 Advanced Course in Photocatalytic Reaction Chemistry 11
12 a game in a two-dimensional lattice Only a unit cell had been shown. like atoms or ions in crystalline lattices unit cell: (in two dimensional lattice) connected to left-right and upper-lowder Unit cell can be moved without change in its size and shape. putting on a lattice point means putting on all the lattice points. 2013/07/11 Advanced Course in Photocatalytic Reaction Chemistry 12
13 unit cell of rutile xyz is as a righthanded x: thumb y: index finger z: mid finger An order of xyz is decided from same length. H a(x =1) x L z Ec(z =1) A A B G O B C C K black: Ti white: O F b(y =1) y J Miller index: William Hallowes Miller unit cell of rutile 2013/07/11 Advanced Course in Photocatalytic Reaction Chemistry 13
14 crystal structure of rutile (1) Q How many TiO 2 s are included in a unit cell? nm (B) red: O green: Ti nm 2013/07/11 Advanced Course in Photocatalytic Reaction Chemistry 14
15 crystal structure of rutile (1) Ti: 1/ = 2 O: 1/ = 4 2TiO nm (B) red: O green: Ti nm 2013/07/11 Advanced Course in Photocatalytic Reaction Chemistry 15
16 crystal structure of rutile (2) Q How many oxygen atoms surround titanium atom (B)? nm (B) red: O green: Ti nm 2013/07/11 Advanced Course in Photocatalytic Reaction Chemistry 16
17 crystal structure of rutile (2) Titanium ion (B) can be divided into 8. Three oxygens for upper or lower 4 unit cells: 6 oxygens nm (B) red: O green: Ti nm 2013/07/11 Advanced Course in Photocatalytic Reaction Chemistry 17
18 coordination numbers Q Show the coordination number of oxygen in TiO 2. The coordination number of oxygen must be 3 when that of titanium is 6 due to the composition of TiO 2. Assuming "octahedron" of oxygen atoms surrounding a titanium atom. 2013/07/11 Advanced Course in Photocatalytic Reaction Chemistry 18
19 squares in octahedron 3 squares can be found in an octahedron 2013/07/11 Advanced Course in Photocatalytic Reaction Chemistry 19
20 octahedron as a basic unit of titania crystals Q Why do all the crystal structures of titania consist of octahedrons? ionic crystals (but not 100%) ratio of ionic radii of Ti 4+ and O 2- is Ti 4+ : nm/o 2- : 0.14 nm 2013/07/11 Advanced Course in Photocatalytic Reaction Chemistry 20
21 radii Q How can we determine the size of atoms, e.g., silicon in its crystal? Q How can we determine the size of ions in ionic crystals? A Size of neutral atoms can be determined knowing the unit cell volume, but size of ions in their ionic crystals. Only sum of sizes of an anion and a cation can be calculated. Therefore, practically, the size of oxygen anion (O 2- ) is assumed to be 0.14 nm, as a consistent value. 2013/07/11 Advanced Course in Photocatalytic Reaction Chemistry 21
22 coordination number r c /r a 2 linear tetrahedral triangle cubic octahedral 2013/07/11 Advanced Course in Photocatalytic Reaction Chemistry 22
23 radius ratio and structure Radius ratio is calculated from the structure. distance between the center and a vertex. 2013/07/11 Advanced Course in Photocatalytic Reaction Chemistry 23
24 coordination numbers Q Show the coordination number of oxygen in TiO 2. The coordination number of oxygen must be 3 when that of titanium is 6 due to the composition of TiO 2. Q How many octahedrons must be connected to one octahedron? (O 2- coordination number: 3) (number of O 2- in an octahedron: 6) (number of coordination in an octahedron: 6) = /07/11 Advanced Course in Photocatalytic Reaction Chemistry 24
25 crystal structure of rutile (3) for octahedron "O": ridge sharing-ab [4] point sharing-defg [4] additional 4 at white vertexes total: 12 octahedron D E A O B F G 2013/07/11 Advanced Course in Photocatalytic Reaction Chemistry 25
26 direction of axis Q Show x, y, and z directions. H a(x =1) x L z Ec(z =1) A A B G O B C C K black: Ti white: O F b(y =1) y J D E A O B F G unit cell of rutile 2013/07/11 Advanced Course in Photocatalytic Reaction Chemistry 26
27 crystal structure of anatase (1) red: O green: Ti nm nm 2013/07/11 Advanced Course in Photocatalytic Reaction Chemistry 27
28 crystal structure of anatase (2) Q How many TiO 2 s are included in a unit cell? A 1 + 4(1/2) + 8(1/8) = 4 <4TiO 2 > Octahedron in anatase is a little skewed. 2013/07/11 Advanced Course in Photocatalytic Reaction Chemistry 28
29 connection of octahedrons in anatase VESTA: database of minerals: /07/11 Advanced Course in Photocatalytic Reaction Chemistry 29
30 sharing of octahedrons in anatase Q How the central octahedron is connected to the other octahedrons? 2013/07/11 Advanced Course in Photocatalytic Reaction Chemistry 30
31 sharing of octahedrons in anatase Q How the central octahedron is connected to the other octahedrons? A Connected to four octahedrons by "ridge" sharing 2013/07/11 Advanced Course in Photocatalytic Reaction Chemistry 31
32 sharing of octahedrons in anatase Q How the central octahedron is connected to the other octahedrons? A Connected to four octahedrons by "ridge" sharing 2013/07/11 Advanced Course in Photocatalytic Reaction Chemistry 32
33 ridge sharing and point (apex) sharing absence of face sharing = impossible to make crystal structure "ridge sharing = 2 additional coordination by a central metal ion "point (apex)" sharing = 1 additional coordination by a central metal ion titanium(iv) oxide = 6 oxygen atoms in an octahedron requires 18 coordination by titanium ions in anatase crystal central titanium ion: 6 4 ridge sharing: 8 (2 each) requiring 4 point sharings 2013/07/11 Advanced Course in Photocatalytic Reaction Chemistry 33
34 ridge sharing and point (apex) sharing absence of face sharing = impossible to make crystal structure "ridge sharing = 2 additional coordination by a central metal ion "point (apex)" sharing = 1 additional coordination by a central metal ion titanium(iv) oxide = 6 oxygen atoms in an octahedron requires 18 coordination by titanium ions in anatase crystal central titanium ion: 6 4 ridge sharing: 8 (2 each) requiring 4 point sharings 2013/07/11 Advanced Course in Photocatalytic Reaction Chemistry 34
35 brookite 8 TiO2 ridge sharing: 3 point sharing: /07/11 Advanced Course in Photocatalytic Reaction Chemistry 35
36 crystal structure of brookite (left) no atoms (ions) at the apexes! (center) VICS and (right) Chime (three dimensional modeling softwares 2013/07/11 Advanced Course in Photocatalytic Reaction Chemistry 36
37 displaying by VESTA (left) displaying by VESTA (lower) a model made of paper 2013/07/11 Advanced Course in Photocatalytic Reaction Chemistry 37
38 comments on this lecture Please send in Japanese or English within 48 hours to: subject: pc xxxxxxxx body: full name nickname comments on this lecture question(s) JPY1,200 (77%) JPY3,500 (79%) pc /07/11 Advanced Course in Photocatalytic Reaction Chemistry 38
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