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Title: Visible-Light-Driven Photocatalytic Z-scheme Overall WaterSplitting in La5Ti2AgS5O7-based Powder Suspension System

Authors: Zhimin Song, Takashi Hisatomi, Shanshan Chen, Qian Wang,Guijun Ma, Shikuo Li, Xiaodi Zhu, Song Sun, and KazunariDomen

This manuscript has been accepted after peer review and appears as anAccepted Article online prior to editing, proofing, and formal publicationof the final Version of Record (VoR). This work is currently citable byusing the Digital Object Identifier (DOI) given below. The VoR will bepublished online in Early View as soon as possible and may be differentto this Accepted Article as a result of editing. Readers should obtainthe VoR from the journal website shown below when it is publishedto ensure accuracy of information. The authors are responsible for thecontent of this Accepted Article.

To be cited as: ChemSusChem 10.1002/cssc.201802306

Link to VoR: http://dx.doi.org/10.1002/cssc.201802306

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Visible-Light-Driven Photocatalytic Z-scheme Overall Water

Splitting in La5Ti2AgS5O7-based Powder Suspension System

Zhimin Song,[a] Takashi Hisatomi,[b] Shanshan Chen,[b] Qian Wang,[b] Guijun Ma,[b] Shikuo Li,[a] Xiaodi

Zhu,[c] Song Sun*[a,c] and Kazunari Domen*[b,d]

Abstract: La5Ti2CuxAg1-xS5O7 (x=0-1) is a kind of long-wavelength-

responsive oxysulfide photocatalysts for hydrogen evolution, and

has been demonstrated to enable the Z-scheme water splitting

coupling with oxygen evolution photocatalysts (OEP) in the

particulate sheet. We herein report that among La5Ti2CuxAg1-xS5O7,

La5Ti2AgS5O7 was found to have the highest performance on Z-

scheme overall water splitting in conjunction with PtOx-WO3 as an

OEP, and a triiodide/iodide (I3−/I

−) redox couple as a shuttle electron

mediator in powder suspension system. Loading Pt/NiS on

La5Ti2AgS5O7 benefits the Z-scheme to achieve an apparent

quantum yield of 0.12% at 420 nm. The finding in powder

suspension system is opposite to the earlier study on photocatalyst

sheet configurations in which p-type doping and the formation of a

solid solution can effectively enhance the water-splitting activity. This

work not only shows a La5Ti2AgS5O7-based Z-scheme water splitting

photocatalyst, but also may present a better understanding for the

difference between particulate sheet and powder suspension system

available in an optimal strategy for water splitting.

Photocatalytic water splitting driven by visible light using

semiconductor materials has been proven as an approach to

sustainable hydrogen generation [1-4]. To effectively use solar

energy, the development of narrow band-gap semiconductors,

such as (oxy)nitrides and (oxy)sulfides, that operate under a

wide range of visible light has been attracting attention [5-8].

However, to date only few photocatalysts capable of overall

water splitting under visible light irradiation have been reported

because of the stringent thermodynamic requirement in the one-

step photoexcitation route [2]. Fortunately Z-scheme

undertaking two-step photoexcitation by combining two functions

of photocatalysts to evolve H2 and O2 separately alleviates the

thermodynamic requirements and expands the choice of

semiconductors [9-11]. In this way a wider range of sunlight

wavelengths can be used. For example, La5Ti2CuxAg1-xS5O7

(x=0-1), one typical kind of oxysulfide semiconductors, exhibiting

intense long-wavelength-response from about 550 nm to 750 nm,

have been demonstrated to show the high photocatalytic activity

in hydrogen evolution, and are promising photocatalysts for Z-

scheme water splitting [12,13]. Recently, our study revealed that

p-type doping and the formation of a Ga3+-La5Ti2Cu0.9Ag0.1S5O7

(Ga-LTCA) solid solution effectively enhance the Z-scheme

water-splitting activity by constructing the photocatalyst sheet

[14]. Similar results were observed in optimized La5Ti2CuS5O7-

based photoelectrodes for photoelectrochemical (PEC) water

splitting as well [15,16]. In other words, Z-scheme particulate

sheet may be partly regarded as the integration of a number of

miniaturized and parallel p/n PEC cells.

However the La5Ti2AgS5O7 (LTA) powders are more active than

La5Ti2CuS5O7 (LTC) and corresponding p-type doping and

La5Ti2CuxAg1-xS5O7 solid solutions in hydrogen evolution

reaction from aqueous solution containing electron donors

(sulphide and sulphite ions) [12]. It implies that Z-scheme water

splitting using oxysulfides in powder suspension system is fairly

controversial when applying the optimization strategy from Z-

scheme sheets or photoelectrodes for PEC water splitting. In

this regard, herein we report the Z-scheme water splitting on the

basis of employing La5Ti2CuxAg1-xS5O7 as a HEP in powder

suspension. As expected, LTA rather than p-type doping or solid

solution samples was found to exhibit the highest Z-scheme

overall water splitting performance in conjunction with WO3 as

an OEP, using a triiodide/iodide (I3−/I−) redox couple as a shuttle

electron mediator in powder suspension. Co-loading Pt and NiS

cocatalysts on LTA promoted the Z-scheme water splitting

activity, with an optimal apparent quantum yield (AQY) of 0.12%

at 420 nm. The results support a comprehensive understanding

for optimization of oxysulfides for Z-scheme water splitting both

in powder suspension system and particulate sheets.

As shown in Figure 1a, the X-ray diffraction (XRD) patterns of

samples indicate that LTA, LTC, La5Ti2Cu0.9Ag0.1S5O7 (LTCA)

and p-type doping Ga-LTCA solid solution were successfully

prepared by a solid-state reaction [15,16]. Relative to LTC, the

major diffraction peaks for LTCA and Ga-LTCA slightly shifted to

lower angles were assigned to the LTC phase, indicating that

samples were not the physical mixture of LTC and LTA, but

formed a solid solution. The similar results were observed over

LTC and LTCA solid solutions in the earlier reports [15,16]. The

UV-vis diffuse reflectance spectra (DRS) of samples (Figure 1b)

[a] Ms. Z. Song, Prof. Dr. S. Li, Prof. Dr. S. Sun.

School of Chemistry and Chemical Engineering

Anhui University

Hefei, Anhui 230601, China

E-mail: suns@ustc.edu.cn

[b] Prof. Dr. T. Hisatomi, Dr. S. Chen, Dr. Q. Wang, Prof. Dr. G. Ma,

Prof. Dr. K. Domen,

Department of Chemical System Engineering, School of

Engineering

The University of Tokyo

7-3-1 Hongo, Bunkyo-ku, Tokyo 113-8656, Japan

E-mail: domen@chemsys.t.u-tokyo.ac.jp

[c] Dr. X. Zhu, Prof. Dr. S. Sun,

National Synchrotron Radiation Laboratory

University of Science and Technology of China

Hefei, Anhui, 230029, China

[d] Prof. Dr. K. Domen,

Center for Energy & Environmental Science, Interdisciplinary Cluster

for Cutting Edge Research

Shinshu University

4-17-1 Wakasato, Nagano-shi, Nagano 380-8553, Japan

Supporting information for this article is given via a link at the end of

the document.

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were also comparable to those obtained in our previous study

[12,15], that substituting Cu for 10% of the Ag shifted the

absorption edge toward longer wavelengths. In addition, Ga3+

doped LTCA shows an absorption edge close to LTCA sample.

Figure 1c and d present the scanning electron microscopy

(SEM) images of LTA sample which is a well-grown columnar

particle. SEM images in Figure S1 revealed that all samples

exhibited columnar particles and that doping or forming solid

solution did not affect the particle morphologies significantly. It

also suggests that p-type doped solid solutions were

synthesized by the solid state reaction in controlled manners.

Figure 1. (a) XRD patterns for LTA, LTC, LTCA, and Ga-LTCA.

The standard XRD patterns for LTA and LTC refer to ICSD

#99613 and #99612, respectively. (b) DRS of LTA, LTC, LTCA,

and Ga-LTCA. (c, d) SEM images of LTA.

Figure 2a shows the photocatalytic H2 evolution rates on LTA,

LTC, LTCA, and Ga-LTCA samples loaded by Pt and NiS, and

co-loaded with Pt and NiS (Pt/NiS). NiS was loaded by in-situ

precipitation [17], while Pt was loaded by the impregnation

method [12]. When NiS and Pt cocatalysts were co-loaded, the

samples were firstly modified with Pt, after which NiS was

loaded onto the Pt-loaded samples by the in-situ precipitation

method. The details of the preparation process are provided in

the Supporting Information. The data of photocatallytic H2

evolution were acquired in aqueous solutions containing Na2S

and Na2SO3 under visible light irradiation. It can be seen that in

each trial using the same cocatalysts, the activities of samples

follow the order of LTA > LTC > LTCA > Ga-LTCA. In contrast to

the performance in PEC systems or particulate sheets that p-

type doping and the formation of a solid solution effectively

enhance the photocatalytic activity [14], the materials without

compositional modifications showed better activities in powder

suspension system. The better acticity of LTA than LTC may

originate from a larger driving force according to the band

structures[12]. Regarding to LTCA, the defects coming from the

formation of solid solution may act as recombination centers of

photogenerated carriers, thereby decreasing the activity.

The optimal loading amount of Pt on 1.0 wt.%-NiS-loaded LTA

was found to be 0.5 wt.%. When varying the NiS amount upon

pre-loading 0.5 wt.% Pt samples, the 1.0 wt.% NiS-loaded LTA

exhibited maximal activity (Figure 2b). The H2 evolution over Pt

(0.5 wt.%)/NiS (1.0 wt.%)-LTA reaches approximately 250

μmol/h which is considerable in comparison to the other representative LTC-based or LTA-based photocatalysts under

sacrificial reagents circumstances [12,17-19] (Figure 2c). It

should be pointed out that Pt is the most effective cocatalyst for

enhancing the hydrogen evolution in comparison to Rh and Ru,

either in loading individual noble metal or in the case of co-

loading M/NiS (M= Rh, Ru, Pt) (Figure 2d). As is well known, the

electron-trapping abilities of noble metals cocatalysts are largely

determined by their work functions which are generally greater

than those of several semiconductors [20]. Thus, it is rational to

explain that Pt with the largest work function among these noble

metals, such as Ru and Rh, is the best candidate cocatalyst for

trapping electrons. On the other hand, although Pt/NiS has been

demonstrated to be effective for improving the H2 evolution over

oxysulfides, it is noteworthy that the enhancement by co-loading

NiS is maximized in the case of Pt/NiS when compared with

Rh/NiS and Ru/NiS (Figure 2d). Besides, the activity of Pt/NiS-

LTA is superior to LTA modified with Pt via photodeposition

process (Figure S2). These results indicated that the

enhancement of Pt/NiS cocatalysis originates from specific

effect between nanoparticulate Pt and amorphous NiS layer.

Figure 2. (a) H2 evolution rates over LTA, LTC, LTCA, and Ga-

LTCA samples loaded with Pt and/or NiS under optimized

conditions. (b) Cocatalyst loading concentration dependent H2

evolution rates over LTA. The blue curve represents loading with

1.0 wt.% NiS and varying amounts of Pt-imp. The green curve

stands for loading with 0.5 wt.% Pt and varying amounts of NiS.

(c) Time course for H2 evolution over LTA loaded with optimal

cocatalyst, 0.5 wt.% Pt and 1.0 wt.% NiS. (d) H2 evolution rates

over LTA loaded with Pt, Ru, and Rh, and followed by co-loading

NiS. The loading amount of noble metal and NiS are 0.5 wt.%,

and 1.0 wt.%, respectively. (a-d) Reaction conditions: 0.2 g of

photocatalyst was loaded with various cocatalysts, 150 mL of an

aqueous 10 mM Na2S and 10 mM Na2SO3 solution, visible light

top irradiation with a 300 W Xe lamp through a cut-off filter (λ>

420 nm).

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Because the H2 evolution on bare NiS was negligible [21], the

significant enhancement in H2 evolution activity of Pt/NiS-LTA

can be attributed to cocatalysis from Pt and NiS. Above all as

shown in Figure 3a, and Figure S3 the close contact of

nanoparticulate Pt and amorphous NiS layer can be clearly

observed on the surface of Pt/NiS-LTA in high resolution

transmission electron microscopy (HR-TEM) image. This

observation is in accord with that in terms of Pt/NiS-LTC [21].

Furthermore, X-ray photoelectron spectroscopy (XPS, Figure

3b) revealed that the co-loading NiS resulted in a slight blue shift

of metallic Pt 4f peak in contrast to only Pt loaded LTA [22]. This

might come from the specific bonding between Pt and NiS.

Likewise, a negligible red shift of Ni 2p is understandable as well

(Figure S4). The XPS of S is not herein referred due to the

existence of S in LTA, which is not in evidence for explaining the

role S in NiS.

Figure 3. (a) HR-TEM image of Pt/NiS-LTA (b) Pt 4f XPS

obtained from Pt-LTA and Pt/NiS-LTA. (c) L3-edge XANES

profiles and (d) Pt L3-edge EXAFS spectra in R space of Pt-LTA

and Pt/NiS-LTA along with a reference of Pt foil.

To further confirm the bonding effect between Pt and NiS,

synchrotron-radiation-based X-ray absorption near-edge

structure (XANES) and extended X-ray absorption fine structure

(EXAFS) were carried out to demonstrate the electronic

structure and coordination information of LTA-based samples.

As shown in Figure 3c, the absorption edge of the samples can

be observed around 11570 eV, reflecting the oxidation states of

Pt species. The similarity in intensity of the jump among Pt-LTA,

Pt/NiS-LTA, and Pt foil indicates that Pt species in Pt-loaded

samples were dominant in metallic state. This observation

agrees well with the result of Pt 4f in XPS tests (Figure 3a).

Moreover, according to Pt L3-edge EXAFS spectra in R space

(Figure 3d), all the samples exhibited only a prominent peak at

2.4 Å, which was attributed to Pt-Pt metallic bonds. It can be

seen that the amplitude of Pt-Pt decreased when NiS was

loaded on the surface of Pt-LTA, revealing the dispersion of NiS

throughout the whole Pt-LTA surface structure. It also

demonstrates that the in-situ precipitation of amorphous NiS

brings up weak bonding between NiS and Pt rather than Pt-S

coordination. Such weak bonding is believed to be superior to

that of Ru/NiS and Rh/NiS, not only serving as effective electron

sinks and providing effective proton reduction sites, but also

facilitating charge transfer from bulk of LTA to the surface of

Pt/NiS. Based on the above analyses, Pt/NiS shows the higher

enhancement of H2 evolution rate when cocatalyzing LTA.

Table 1. The photocatalytic water splitting activities of LTA-

based or LTC-based oxysulfide as the HEP and PtOx-WO3 as an

OEP.

Entry HEP OEP a

Activity (µmol h−1) b

H2 O2

1 LTA WO3 0.1 c trace

2 Pt-LTA WO3 5.6 2.6

3 NiS-LTA WO3 2.3 c 1.1 c

4 Pt/NiS-LTA WO3 11.1 5.4

5 Pt/NiS-LTC WO3 7.5 3.7

6 Pt/NiS-LTCA WO3 3.7 1.8

7 Pt/NiS-Ga-LTCA WO3 1.9 0.9

8 d Pt/NiS-LTA WO3 not detected not detected

9 Pt/NiS-LTA --- 1.0 c not detected

10 --- WO3 not detected trace a All the WO3 in this table were pre-treated by H

+ and Cs

+, and

loaded 0.5 wt.% PtOx (see Figure S5). b Reaction conditions: 0.05 g HEP; 0.15 g OEP; 150 mL NaI

aqueous solution (2.5 mM); light source: 300 W Xe lamp equipped

with a visible light filter (λ > 420 nm). c observed only in the initial few hours.

d no redox mediator was used in this entry.

On the basis of excellent H2 evolution activity of Pt/NiS loaded

LTA, we further explored the visible light-induced Z-scheme

water splitting by using Pt/NiS-LTA as the HEP. Although BiVO4

has been demonstrated as an efficient OEP in Z-scheme water

splitting in the form of particulate sheet, it is missing to show

activity in powder suspension in conjunction with LTA-based

(Table S1) photocatalysts as a HEP either using I3−/I− or

Fe3+/Fe2+ as an electron mediator. One reason is that Fe3+/Fe2+

is prone to be active in acid circumstances, which is harmful to

oxysulfides for degrading or dissolving surface sulfur species

[23]. While the backward reaction, oxidation of I− to I3− (or IO3

−)

preferentially proceeds over the BiVO4 photocatalyst instead of

the oxidation of water [23, 24]. It is also partly due to that Z-

scheme sheet can be regarded as a miniaturized and parallel

p/n PEC cell in a broad sense that functions under the

photocurrent cross-point of photocathode and photoanode [25].

Therefore the optimization in powder suspension system on

performance enhancement is opposite to the previous studies

on photocatalyst sheet configurations in which p-type doping

and the formation of a solid solution can effectively enhance the

water-splitting activity.

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Our earlier study reported the Z-scheme water splitting by

utilizing WO3 as an OEP at neutral pH, which encouraged us to

apply WO3 to the present oxysulfide-based Z-scheme water

splitting systems [13]. An efficient O2 evolution was obtained

over WO3 with different treatments and cocatalyst (Figure S5).

As expected, both the H2 and O2 evolution activities were

observed under visible light irradiation (Table 1). The decrease

of activities over the p-type doping and solid solutions samples

(entry 6 and 7, Table 1) further confirmed that the optimization

strategy in Z-scheme sheets or photoelectrodes for PEC water

splitting is fairly controversial with that in powder suspension

system. During the prolonged trial (Figure 4), the apparatus was

evacuated in first 2 h to remove the produced gases. The H2/O2

ratio was evidently closer to 2 after this operation. The AQY of

the system was estimated to be 0.12% at 420 nm, which is lower

than in oxysulfides-constructed Z-scheme particulate

photocatalyst sheet, but is still considerable in oxysulfides-based

powder suspension system [13,19]. Following a reaction time of

8 h, 70% of the initial photocatalytic activity was maintained. The

deactivation may not come from shuttle electron mediators [13],

but rather photocorrosion by photogenerated holes that are not

consumed timely.

Figure 4. Time course of Z-scheme water splitting using Pt/NiS-

LTA as a HEP, 0.5 wt.% PtOx-loaded WO3 as an OEP, and I3−/I−

as a shuttle electron mediator under visible light irradiation.

Catalysts, 0.05 g Pt/NiS-LTA and 0.15 g PtOx-WO3; 150 mL NaI

aqueous solution (2.5 mM) with a pH of 4.0; light source, 300 W

Xe lamp with a cutoff filter (λ > 420 nm).

In summary, the synthesis of LTA by the solid state method and

subsequent co-loading with Pt and NiS to generate efficient

reduction sites, were found to be essential for enhancing the H2

evolution activity of LTA and thereby increasing the water

splitting activity of the Z-scheme system. The performance

comparison concluded that the strategies on performance

enhancement in photocatalyst sheets or PEC systems are not

applicable to the optimization in powder suspension system.

Visible light-driven Z-scheme water splitting using Pt/NiS-LTA as

the HEP, surface treated WO3 as an OEP, and the I3−/I− ion

couple as a redox mediator, achieved an AQY of 0.12% at 420

nm. This work demonstrates that narrow band gap oxysulfide

photocatalysts can be applied to obtain effective visible light-

driven Z-scheme water splitting through promotion of the H2

evolution activity. The finding also expands understandings for

optimization strategy for Z-scheme water splitting in powder

suspension system.

Experimental Section

Experimental Details are presented in the Supporting Information.

Acknowledgements

This work was financially supported by the National Key

Research and Development Program of China (No.

2016YFB0700205), the National Natural Science Foundation of

China (U1632273, U1832165) and Foundation from Key

Laboratory of Photovoltaic and Energy Conservation, CAS

(PECL2018KF012). A part of this work was supported by the

Artificial Photosynthesis Project of the New Energy and

Industrial Technology Development Organization (NEDO) and

by Grants-in-Aids for Scientific Research (A) (No. 16H02417)

and for Young Scientists (A) (No. 15H05494) from the Japan

Society for the Promotion of Science (JSPS). The authors

acknowledge the technical supports from the BL11U beamline in

National Synchrotron Radiation Laboratory (NSRL,China) and

the 1W1B beamline of the Beijing Synchrotron Radiation Facility

(BSRF, China), respectively, in acquiring XPS and EXAFS data.

Keywords: water splitting • Z-scheme • photocatalysis •

oxysulfides • visible light

Current affiliation: Takashi Hisatomi and Shanshan Chen,

Center for Energy & Environmental Science, Interdisciplinary

Cluster for Cutting Edge Research, Shinshu University, 4-17-1

Wakasato, Nagano-shi, Nagano 380-8553, Japan; Qian Wang,

Department of Chemistry, University of Cambridge, Lensfield

Road, Cambridge, CB2 1EW, UK; Guijun Ma, School of Physical

Science and Technology, Shanghai Tech University, Shanghai

201210, China.

References

[1] N. Lewis, Science 2016, 351, aad1920.

[2] A. Kudo, Y. Miseki, Chem. Soc. Rev. 2009, 38, 253-278. [3] X. Chen, L. Liu, P. Yu, S. Mao, Science. 2011, 331, 746-

750.

[4] F. Osterloh, Chem. Soc. Rev. 2013, 42, 2294-2320. [5] Z. Wang, Y. Inoue, T. Hisatomi, R. Ishikawa, Q. Wang, T.

Takata, S. Chen, N. Shibata. Y. Ikuhara, K. Domen, Nat.

Catal. 2018, DOI: 10.1038/s41929-018-0134-1. [6] D. Lu, T. Takata, N. Saito, Y. Inoue, K. Domen, Nature.

2006, 440, 295.

[7] X. Wang, K. Maeda, X. Chen, K. Takanabe, K. Domen, Y. Hou, X. Fu, M. Antonietti, J. Am. Chem. Soc. 2009, 131, 1680-1681.

10.1002/cssc.201802306

Acc

epte

d M

anus

crip

t

ChemSusChem

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COMMUNICATION

[8] C. Wolff, P. Frischmann, M. Schulze, B. Bohn, R. Wein, P. Livadas, M. Carlson, F. Jäckel, J. Feldmann, F. Würthner,

J. Stolarczyk, Nat. Energy 2018, DOI: 10.1038/s41560-018-0229-6.

[9] H. Li, W. Tu, Y. Zhou, Z. Zou, Adv. Sci. 2016, 3, 1500389.

[10] T. Hisatomi, J. Kubota, K. Domen, Chem. Soc. Rev. 2014, 43, 7520-7535.

[11] S. Chen, T. Takata, K. Domen, Nat. Rev. Mater. 2017, 2,

17050. [12] T. Suzuki, T. Hisatomi, K. Teramura, Y. Shimodaira, H.

Kobayashi. K. Domen, Phys. Chem. Chem. Phys. 2012, 14,

15475-15481. [13] G. Ma, S. Chen, Y. Kuang, S. Akiyama, T. Hisatomi, M.

Nakabayashi, N. Shibata, M. Katayama, T. Minegishi, K.

Domen, J. Phys. Chem. Lett. 2016, 7, 3892-3896. [14] S. Sun, T. Hisatomi, Q. Wang, S. Chen, G. Ma, J. Liu, S.

Nandy, T. Minegishi. M. Katayama, K. Domen, ACS. Catal.

2018, 8, 1690-1696. [15] T. Hisatomi, S. Okamura, J. Liu, Y. Shinohara, K. Ueda, T.

Higashi, M. Katayama, T. Minegishi, K. Domen, Energy

Environ. Sci. 2015, 8, 3354-3362. [16] J. Liu, T. Hisatomi, G. Ma, A. Iwanaga, T. Minegishi, Y.

Moriya, M. Katayama, J. Kubota, K. Domen, Energy

Environ. Sci. 2014, 7, 2239-2242. [17] S. Nandy, Y. Goto, T. Hisatomi, Y. Moriya, T. Minegishi, M.

Katayama, K. Domen, ChemPhotoChem. 2017, 1, 1-9.

[18] M. Katayama, D. Yokoyama, Y. Maeda, Y. Ozaki, M. Tabata, Y. Matsumoto, A. Ishikawa, J. Kubota, K. Domen, Materials Science and Engineering B, 2010,173, 275-278.

[19] S. Nandy, T. Hisatomi, S. Sun. M. Katayama, T. Minegishi, K. Domen, ACS Appl. Mater. Interfaces 2018, DOI: 10.1021/acsami.8b02909

[20] J. Yang, D. Wang, H. Han, C. Li, Acc. Chem. Res. 2013, 46, 1900-1909.

[21] S. Nandy, T. Hisatomi, G. Ma. T. Minegishi, M. Katayama,

K. Domen, J. Mater. Chem. A. 2017, 5, 6106-6112. [22] J. Kim, J. Cheon, T. Shin, J. Pak, S. Joo, Carbon 2016,

101, 449-457.

[23] Nanostructured photocatalysts, Advanced Functional Materials, Hiraomi Yamashita, Hexing Li editors, book published by Springer International Publishing Switzerland

2016. [24] R. Abe, K. Sayama, H. Sugihara, J. Phys. Chem. B 2005,

109, 16052-16061.

[25] Q. Wang, T. Hisatomi, Y. Suzuki, Z. Pan, J. Seo, M. Katayama, T. Minegishi, H. Nishiyama, T. Takata, K. Seki, A. Kudo, T. Yamada, K. Domen, J. Am. Chem. Soc. 2017,

139, 1675-1683

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Visible light-driven Z-scheme water

splitting using Pt/NiS loaded LTA as

the HEP, PtOx-WO3 as an OEP,

and the I3−/I− as the redox mediator,

achieved an AQY of 0.12% at 420

nm. This work demonstrated that

the optimization strategy for Z-

scheme water splitting in powder

suspension system is different from

that in particulate photocatalyst

sheets or PEC system.

Zhimin Song,[a] Takashi Hisatomi,[b]

Shanshan Chen,[b] Qian Wang,[b]

Guijun Ma,[b] Shikuo Li,[a] Xiaodi

Zhu,[c] Song Sun*[a,c] and Kazunari

Domen*[b,d]

Page No. – Page No.

Visible-Light-Driven

Photocatalytic Z-scheme Overall

Water Splitting in La5Ti2AgS5O7-

based Powder Suspension

System

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