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Supporting information
Preparation and Catalytic Activity for Aerobic Glucose Oxidation of Crown Jewel Structured Pt/Au Bimetallic Nanoclusters

Haijun Zhang1*, Liqiong Wang1, Lilin Lu1, and Naoki Toshima2*



1The State Key Laboratory of Refractories and Metallurgy, Wuhan University of Science and Technology, Wuhan 430081, China

2Department of Applied Chemistry, Tokyo University of Science Yamaguchi, SanyoOnoda, Yamaguchi 756-0884, Japan
*Corresponding author;

E-mail of the corresponding author:

Prof. Haijun Zhang: zhanghaijun@wust.edu.cn;

Prof. Naoki Toshima: toshima@rs.tus.ac.jp;



Table S1 Preparation conditions of CJ-Pt/Au NCs by replacement reaction method

Code

Preparation conditions of Au atom

Pt/Au3+, atom ratio

Conditions

CJ-1

55/3

100C/30 min

CJ -2

55/6

100C/30 min

CJ -3

55/12

100C/30 min

CJ -4

55/18

100C/30 min

CJ -5

55/38

100C/30 min

CJ -6

55/46

100C/30 min

CJ -7

55/73

100C/30 min

3Pt + 4Au3+ = 4Au + 3Pt4+
Table S2 Theoretical lattice spacing of bulk Au and Pt with various reflection planes.

Reflection plane

Lattice spacing, nm

Au

Pt

(111)

0.2355

0.2265

(200)

0.2040

0.1962

(220)

0.1442

0.1387

(311)

0.1230

0.1183

(222)

0.1178

0.1133

(Au: JCPDS 89-3697; Pt: JCPDS 04-0802)

Table S3 Lattice spacing and indexed reflection planes of CJ-2 and CJ-3 BNCs determined by HR-TEM

Samples

Measured Lattice

spacing, nm



Remarks

Indexed reflection plane of the BNCs

CJ-2

0.227

In the range of Au(111) and Pt(111)

(111)

CJ-3

0.229

In the range of Au(111) and Pt(111)

(111)


Table S4 Comparison of theoretical and measured Au contents of the prepared CJ-Pt/Au NCs.

Code

Theoretical contents

ICP contents, mol

Starting

Pt/Au3+, mol



Theoretical Au content, wt%

Final

Au%, wt%


CJ-1

55/3

5.37

5.31

CJ -2

55/6

10.60

8.87

CJ -3

55/12

20.65

16.53

CJ -4

55/18

30.19

22.83

CJ -5

55/38

58.79

38.61

CJ -6

55/46

69.05

56.82

CJ -7

55/73

100

66.67

3Pt + 4Au3+ = 4Au + 3Pt4+

(a) HRTEM



(b) TEM-mapping EDS



(c) TEM micrograph and size distribution



Figure S1. HRTEM (a), mapping EDS (b), and TEM micrograph and size distribution (c) of Pt mother clusters prepared by rapid injection of NaBH4 (1.32mM, RPVP=100).



Figure S2. The NaOH amount -time curve for glucose oxidation over “top Au atoms supported on Pt clusters” catalyst prepared by replacement reaction (CJ-2) and a fit straight line for determining TOF (Glucose/Au=36500, mol ratio; O2: 100ml/min; about 0.0020g catalyst was used for evaluation.).


(a) CJ-2


(b) CJ-3

Figure S3. TEM and mapping EDS of CJ-2 and CJ-3 BNCs

(a) CJ-2 (b) CJ-3



Figure S4. HRTEM micrograph of CJ-2 and CJ-3 BNCs

(a) CJ-1 (b) CJ-2



(c) CJ-3 (d) CJ-4



(f) CJ-5 (g) CJ-6



(h) CJ-7


Figure S5. Size distribution of CJ-Pt/Au BNCs series catalysts prepared by replacement reaction method.


Figure S6. HADDF-STEM images of a CJ-Pt/Au BNC (The red circle in the images indicates the presence of the vacancy resulted from replacement reaction process between Pt mother clusters and Au3+ ions. The green dashed square indicates the shape of the NC.).

(a) XPS spectrum of CJ-3 BNCs



(b) Au 4f (c) Pt 4f



Figure S7. Au 4f and Pt 4f XPS core level spectra recorded from CJ-3 BNCs (RPVP=100).
References

[S1] H. J. Zhang, T. Watanabe, M. Okumura, M. Haruta, N. Toshima, Nature Mater., 2012, 11, 49-52.



[S2] H. J. Zhang, L. L, Lu, K, Kawashima, M, Okumura, M, Haruta, N, Toshima, Adv. Mater., 2015, 27(8): 1383-1388.







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