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Tio2 As a Photocatalyst for Water Splitting—An Experimental and Theoretical Review

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Tio2 As a Photocatalyst for Water Splitting—An Experimental and Theoretical Review molecules Review TiO2 as a Photocatalyst for Water Splitting—An Experimental and Theoretical Review Håkon Eidsvåg 1,* , Said Bentouba 1, Ponniah Vajeeston 2, Shivatharsiny Yohi 3 and Dhayalan Velauthapillai 1,* 1 Department of Computing, Mathematics and Physics, Western Norway University of Applied Sciences, Inndalsveien 28, Box 5063, N-5009 Bergen, Norway; [email protected] 2 Center for Materials Science and Nanotechnology, Department of Chemistry, University of Oslo, Box 1033 Blindern, N-0315 Oslo, Norway; [email protected] 3 Department of Chemistry, Faculty of Science, University of Jaffna, Sir. Pon, Ramanathan Rd, Jaffna 40000, Sri Lanka; [email protected] * Correspondence: [email protected] (H.E.); [email protected] (D.V.); Tel.: +47-980-61-444 (H.E.); +47-55-58-77-11 (D.V.) Abstract: Hydrogen produced from water using photocatalysts driven by sunlight is a sustainable way to overcome the intermittency issues of solar power and provide a green alternative to fossil fuels. TiO2 has been used as a photocatalyst since the 1970s due to its low cost, earth abundance, and stability. There has been a wide range of research activities in order to enhance the use of TiO2 as a photocatalyst using dopants, modifying the surface, or depositing noble metals. However, the issues such as wide bandgap, high electron-hole recombination time, and a large overpotential for the hydrogen evolution reaction (HER) persist as a challenge. Here, we review state-of-the-art experimental and theoretical research on TiO2 based photocatalysts and identify challenges that Citation: Eidsvåg, H.; Bentouba, S.; have to be focused on to drive the field further. We conclude with a discussion of four challenges Vajeeston, P.; Yohi, S.; Velauthapillai, for TiO2 photocatalysts—non-standardized presentation of results, bandgap in the ultraviolet (UV) D. TiO2 as a Photocatalyst for Water region, lack of collaboration between experimental and theoretical work, and lack of large/small Splitting—An Experimental and scale production facilities. We also highlight the importance of combining computational modeling Theoretical Review. Molecules 2021, with experimental work to make further advances in this exciting field. 26, 1687. https://doi.org/10.3390/ molecules26061687 Keywords: TiO2; water-splitting; theoretical; experimental; DFT Academic Editor: Smagul Karazhanov Received: 2 February 2021 1. Introduction Accepted: 10 March 2021 Over the last years, there has been a steadily increasing focus on clean, renewable Published: 17 March 2021 energy sources as a priority to hinder the irreversible climate change the world is facing and to meet the continuously growing energy demand [1]. One hour of solar energy can satisfy Publisher’s Note: MDPI stays neutral the energy consumption of the whole world for a year [2]. Hence, direct harvesting of solar with regard to jurisdictional claims in light and its conversion into electrical energy with photovoltaic cells or chemical energy published maps and institutional affil- by photoelectrochemical reactions are the most relevant technologies to overcome this iations. challenge. Conventionally, both technologies rely on the collection of light in semiconductor materials with appropriate bandgaps matching the solar spectrum, and thus providing a high-energy conversion efficiency. Unfortunately, the technology has drawbacks, which prevent it from overtaking Copyright: © 2021 by the authors. non-renewable energy as the main energy source. A major issue is the uneven power Licensee MDPI, Basel, Switzerland. distribution caused by varying solar radiation and a lack of proper storage alternatives. This article is an open access article As a solution to this problem, the focus is moving toward research on storage options distributed under the terms and for the produced electricity, which we can divide into mechanical and electrochemical conditions of the Creative Commons storage systems. For example, in Oceania, pumped hydroelectricity (mechanical) is the Attribution (CC BY) license (https:// most common storage system for excess electricity [3]. Different batteries (lithium–ion, creativecommons.org/licenses/by/ sodium–sulfur (S), vanadium, etc.), hydrogen fuel cells, and supercapacitors are the current 4.0/). Molecules 2021, 26, 1687. https://doi.org/10.3390/molecules26061687 https://www.mdpi.com/journal/molecules Molecules 2021, 26, 1687 2 of 30 MoleculesMolecules 2021 2021, 26, ,26 x ,FOR x FOR PEER PEER REVIEW REVIEW 2 of2 of30 30 areas for electrochemical storage [3]. There are several reasons for choosing hydrogen as areasfocus areasfor electrochemical for electrochemical storage storage [3]. There [3]. There are several are several reasons reasons for forchoosing choosing hydrogen hydrogen as a way to store solar energy, namely, (1) there is a high abundance of hydrogen from re- aas way a way to store to store solar solar energy, energy, namely, namely, (1) (1)there there is a is high a high abundance abundance of hydrogen of hydrogen from from re- newable sources; (2) it is eco-friendly when used; (3) hydrogen has a high-energy yield, newablerenewable sources; sources; (2) (2) it itis is eco-friendly eco-friendly when when used; used; (3) (3) hydrogen hydrogen ha hass a a high-energy high-energy yield, and (4) it is easy to store as either a gas or a liquid [4–6]. and (4) it is easy to store as either a gas or a liquid [[4–6].4–6]. TheThe high high energy energy yield yield and and ease ease of ofstorage storage make make hydrogen hydrogen viable viable as asfuel fuel for for the the long long transporttransport sector; sector; airplanes, airplanes, cruise cruise ships, ships, traile trailers,trailers,rs, and and cargo cargo ships shipsships [7,8]. [[7,8].7,8 The]. The realization realization of ofa a greengreen energy energy shipping shipping fleet fleetfleet could could alone alone yearly yearly cut cut 2.5% 2.5% of of ofglobal globalglobal greenhouse greenhousegreenhouse emissions emissionsemissions (GHG)(GHG) [9]. [[9].9 However,]. However, However, to to succeed succeed in in this this stra stra strategy,tegy,tegy, hydrogen hydrogenhydrogen must must be be produced producedproduced in ina clean aa cleanclean andand renewable renewable way. way. AsAs water water splitting splitting got got the the attention attention of ofthe the researchers researchers in inthe the 1970s, 1970s,1970s, titanium titaniumtitanium dioxide dioxidedioxide becamebecame the the most most prominent prominent photocatalyst photocatalyst used used [10]. [[10].10 There]. There are are several several good good reasons reasons for forfor this: low cost, chemical stability, earth abundance, and nontoxicity [11]. However, TiO2 this: lowlow cost,cost, chemicalchemical stability, stability, earth earth abundance, abundance, and and nontoxicity nontoxicity [11]. [11]. However, However, TiO2 TiOalso2 alsoalsosports sports sports a wide a widea wide bandgap bandgap bandgap (3.0–3.2 (3.0–3.2 (3.0–3.2 eV), eV), which eV), which which reduces reduces reduces the potentialthe the potential potential for absorption for for absorption absorption of visible of of 2 visiblevisiblelight light [11 light]. [11]. Due [11]. Due to Due TiO to to2TiOs TiO structurals 2structurals structural and and chemical and chemical chemical properties, properti properties, ites, isit possible isit possibleis possible to to engineer toengineer engineer the thethebandgap, bandgap, bandgap, light light light absorption absorption absorption properties, properties, properties, recombination recombination recombination time, time, time, etc. etc. by etc. by increasing by increasing increasing the the active the active active sites sitessitesand and improvingand improving improving the the electrical the electrical electrical conductivity conductivity conductivity [12]. [12]. TiO [12]. 2TiOexists TiO2 exists2 inexists several in inseveral several different different different polymorphs poly- poly- morphsmorphsthat all that behavethat all all behave differently.behave differently. differently. The most The The most common most common common ones ones are ones rutile, are are rutile, brookite,rutile, brookite, brookite, and and anatase and ana- ana- as tasetaseshown as asshown inshown Figure in inFigure1 Figure. Rutile 1. 1.Rutile and Rutile anatase and and anatase TiOanatase2 are TiO TiO the2 are most2 are the the used most most polymorphs used used polymorphs polymorphs for photocatalytic for for pho- pho- tocatalyticwatertocatalytic splitting; water water splitting; nevertheless, splitting; nevertheless nevertheless some attempts, some, some withattempts attempts amorphous with with amorphous amorphous TiO2 (aTiO TiO2 TiO) have2 (aTiO2 (aTiO been2) have2) made have beenbeenas shownmade made as in asshown Figure shown 2in. inFigure Figure 2. 2. Figure 1. Crystal structures of TiO rutile (tetragonal, P42/mmm), brookite (orthorhombic, Pbca), FigureFigure 1. Crystal1. Crystal structures structures of ofTiO TiO2 rutile22 rutile (tetragonal, (tetragonal, P42/mmm), P42/mmm), brookite brookite (orthorhombic, (orthorhombic, Pbca), Pbca), andand anatase anatase (tetragonal, (tetragonal, I41/amd) I41/amd) pol pol polymorphs.ymorphs.ymorphs. Reused Reused Reused with with with permission permission permission from from from [13] [13] [13. ].. Figure 2. The structure of 72-atom (left), 96-atom (middle), and 216-atoms (right) models of amorphous TiO2. The red and FigureFigure 2. The2. The structure structure of of72-atom 72-atom (left), (left), 96-atom 96-atom (middle) (middle),
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