Key Laboratory of Material Chemistry for Energy Conversion and Storage (Ministry

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Electronic Supplementary Material (ESI) for Dalton Transactions. This journal is The Royal Society of Chemistry 2018 Supporting Information for Dramatically enhanced visible-light driven H 2 evolution by anchoring TiO 2 nanoparticles on the molecularly grafted carbon nitride nanosheets via a multiple modification strategy Jingyu Wang,* a Zili Xu, a Chuansheng Zhuang, b Heng Wang, a Xiaochan Xu, a Bien Tan, a Tao Li,* a and Tianyou Peng* b a Key Laboratory of Material Chemistry for Energy Conversion and Storage (Ministry of Education), School of Chemistry and Chemical Engineering, Huazhong University of Science and Technology, Wuhan 430074, Hubei, China. E-mail: wangjingyu@hust.edu.cn; taoli@mail.hust.edu.cn. b College of Chemistry and Molecular Sciences, Wuhan University, Wuhan 430072, P. R. China. E-mail: typeng@whu.edu.cn.

Figures Figure S1. XRD patterns of bulk CN, bulk CNX, and CNX-NSs. Figure S2. TGA curve of the TiO 2 /CNX-NSs hybrid with the theoretical mass ratio of TiO 2 to CNX-NSs at 1:3.

Figure S3. SEM (a) and TEM (b) images of bulk CNX. Figure S4. TEM image of TiO 2 hydrosol.

Figure S5. The XPS survey spectra of bulk CNX, CNX-NSs, TiO 2, and TiO 2 /CNX- NSs (3:1) hybrid. Figure S6. Comparison of UV-vis DRS of CN materials before and after liquid-phase exfoliation.

Figure S7. The transient-state photoluminescence decay spectra of bulk CN (a), bulk CNX (b), TiO 2 (c), and TiO 2 /CNX-NSs hybrid (d).

Figure S8. UV-Vis transmittance spectrum of the 400 nm cutoff filter that installed outside the 300 W Xe lamp. Figure S9. Wavelength-dependent AQY of H 2 production by the TiO 2 /CN-NSs hybrid using the correspondingband-pass filters of λ ± 15 nm. The UV vis DRS is overlapped for comparison.

Figure S10. XRD patterns of the TiO 2 /CNX-NSs hybrid before and after cycles of photocatalytic reaction. Figure S11. FT-IR spectra of the TiO 2 /CNX-NSs hybrid before and after cycles of photocatalytic reaction.

Table S1. Decay lifetimes related to the transient-state photoluminescence spectra of bulk CN, bulk CNX, TiO 2, and TiO 2 /CNX-NSs hybrid. Samples τ 1 (ns) A 1 (%) τ 2 (ns) A 2 (%) < τ > (ns) bulk CN 2.16 52.51 8.45 47.49 7.06 bulk CNX 1.51 51.95 6.55 48.05 5.55 TiO 2 1.36 61.37 9.58 38.63 8.07 TiO 2 /CNX- 0.50 49.29 2.73 50.71 2.39 NSs The average lifetime could be calculated by the following equation: < τ >= A 1 τ2 1 + A 2 τ2 2 A 1 τ 1 + A 2 τ 2 Where <τ>, τ and A represent the intensity-average lifetime, decay time and relative magnitude of components, respectively.

Table S2. Comparisons of H 2 production rate with the analogue photocatalysts in the recent literatures. Photocatalyst (mg) Co-catalyst Light source Scavenger H 2 (μmol/h) AQY Ref C-TiO 2 /g-c 3 N 4 50 Pt 300W Xe lamp ( 420 nm) N-TiO 2 /g-c 3 N 4 3 - Xenon lamp ( 420 nm) g-c 3 N 4 /TiO 2 100 Pt 300W Xe lamp TiO 2 @g-c 3 N 4 nanospheres ( 420 nm) 10-300W Xe lamp ( 420 nm) 3D g-c 3 N 4 /TNA 100 Pt 300W Xe lamp ( 400 nm) g-c 3 N 4 /TiO 2 45 Pt 800W Xe-Hg lamp( 420nm) g-c 3 N 4 /TiO 2 100 Pt 500W Xe lamp g-c 3 N 4 /TiO 2 Nanofibers (>420 nm) 5 Ag 300W Xe lamp ( 400 nm) g-c 3 N 4 /Ni 3 C 50 Ni 3 C 350W Xe lamp (>420 nm) Ni 12 P 5 /g-c 3 N 4 50 Ni 12 P 5 350W Xe lamp (>420 nm) NiS/g-C 3 N 4 50 NiS 350W Xe lamp g-c 3 N 4 /carbon /NiS (>420 nm) 50 NiS 300W Xe lamp ( 420 nm) g-c 3 N 4 -Ni-NiS 50 Ni/NiS 300W Xe lamp (>420 nm) NiS/g-C 3 N 4 50 Pt 300W Xe lamp /SrTiO 3 ( 420 nm) Na-doped g- 50 Pt 350W Xe lamp C 3 N 4 (>400 nm) WO 3 /g-c 3 N 4 50 Ni(OH) x 300W Xe lamp /Ni(OH) x (>400 nm) g-c 3 N 4 /Ag-SCN 50 Ag-SCN 3W LED (420 nm) TiO 2 /CNX-NSs 50 Pt 300W Xe lamp ( 400 nm) TEOA 57.28 6.2% at 420 nm methanol 0.89 1.2% at 420nm [1] [2] TEOA 68.76 - [3] methanol 0.356 - [4] methanol 24.3 - [5] TEOA 1.35 - [6] methanol 35.44 - [7] TEOA 0.305 - [8] TEOA 15.18 0.40% at 420 nm [9] TEOA 6.33 - [10] TEOA 29.68 [11] TEOA 18.32 - [12] TEOA 25.75 [13] methanol 86.135 - [14] TEOA 18.7 - [15] TEOA 28.8 - [16] lactic acid 3.89 - [17] TEOA 138.4 7.1±0.2% at 450 nm This work

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