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Showing papers by "Jiaguo Yu published in 2018"


Journal ArticleDOI
TL;DR: In this article, a review summarizes the recent significant progress on the design of g-C3N4-based heterostructured photocatalysts and their special separation/transfer mechanisms of photogenerated charge carriers.
Abstract: Photocatalysis is considered as one of the promising routes to solve the energy and environmental crises by utilizing solar energy. Graphitic carbon nitride (g-C3N4) has attracted worldwide attention due to its visible-light activity, facile synthesis from low-cost materials, chemical stability, and unique layered structure. However, the pure g-C3N4 photocatalyst still suffers from its low separation efficiency of photogenerated charge carriers, which results in unsatisfactory photocatalytic activity. Recently, g-C3N4-based heterostructures have become research hotspots for their greatly enhanced charge carrier separation efficiency and photocatalytic performance. According to the different transfer mechanisms of photogenerated charge carriers between g-C3N4 and the coupled components, the g-C3N4-based heterostructured photocatalysts can be divided into the following categories: g-C3N4-based conventional type II heterojunction, g-C3N4-based Z-scheme heterojunction, g-C3N4-based p–n heterojunction, g-C3N4/metal heterostructure, and g-C3N4/carbon heterostructure. This review summarizes the recent significant progress on the design of g-C3N4-based heterostructured photocatalysts and their special separation/transfer mechanisms of photogenerated charge carriers. Moreover, their applications in environmental and energy fields, e.g., water splitting, carbon dioxide reduction, and degradation of pollutants, are also reviewed. Finally, some concluding remarks and perspectives on the challenges and opportunities for exploring advanced g-C3N4-based heterostructured photocatalysts are presented.

1,759 citations



Journal ArticleDOI
TL;DR: In this article, a review concisely compiles the recent progress in the fabrication, modification, and major applications of the direct Z-scheme photocatalysts; the latter include water splitting, carbon dioxide reduction, degradation of pollutants, and biohazard disinfection.

1,013 citations


Journal ArticleDOI
TL;DR: This work reports a new metal-free phosphorene/g-C3 N4 photocatalyst and sheds lights on the design and fabrication of 2D/2D VDW heterojunction for applications in catalysis, electronics, and optoelectronics.
Abstract: The generation of green hydrogen (H2 ) energy using sunlight is of great significance to solve the worldwide energy and environmental issues. Particularly, photocatalytic H2 production is a highly promising strategy for solar-to-H2 conversion. Recently, various heterostructured photocatalysts with high efficiency and good stability have been fabricated. Among them, 2D/2D van der Waals (VDW) heterojunctions have received tremendous attention, since this architecture can promote the interfacial charge separation and transfer and provide massive reactive centers. On the other hand, currently, most photocatalysts are composed of metal elements with high cost, limited reserves, and hazardous environmental impact. Hence, the development of metal-free photocatalysts is desirable. Here, a novel 2D/2D VDW heterostructure of metal-free phosphorene/graphitic carbon nitride (g-C3 N4 ) is fabricated. The phosphorene/g-C3 N4 nanocomposite shows an enhanced visible-light photocatalytic H2 production activity of 571 µmol h-1 g-1 in 18 v% lactic acid aqueous solution. This improved performance arises from the intimate electronic coupling at the 2D/2D interface, corroborated by the advanced characterizations techniques, e.g., synchrotron-based X-ray absorption near-edge structure, and theoretical calculations. This work not only reports a new metal-free phosphorene/g-C3 N4 photocatalyst but also sheds lights on the design and fabrication of 2D/2D VDW heterojunction for applications in catalysis, electronics, and optoelectronics.

683 citations


Journal ArticleDOI
TL;DR: In this paper, a rice crust-like structure was achieved through the uniform distribution of TiO2 nanoparticles on MXene Ti3C2 through calcination method and a unique rice crustlike structure of the prepared samples rendered the composite with large population of the surface active sites.

557 citations


Journal ArticleDOI
TL;DR: In this article, a 2D/2D g-C3N4/MnO2 heterostructured photocatalyst was synthesized via in situ growth of MnO2 nanosheets on the surface of G-C 3N4 nanolayers using a wet-chemical method.
Abstract: Constructing two-dimensional (2D) composites using layered materials is considered to be an effective approach to achieve high-efficiency photocatalysts. Herein, a 2D/2D g-C3N4/MnO2 heterostructured photocatalyst was synthesized via in situ growth of MnO2 nanosheets on the surface of g-C3N4 nanolayers using a wet-chemical method. The hybrid nanomaterial was characterized by a range of techniques to study its micromorphology, structure, chemical composition/states, and so on. The g-C3N4/MnO2 nanocomposite exhibited greatly improved photocatalytic activities for dye degradation and phenol removal in comparison to the single g-C3N4 or MnO2 component. On the basis of the electron paramagnetic resonance spectra, X-ray photoelectron spectra, and the Mott–Schottky measurements, we consider that a Z-scheme heterojunction was generated between the g-C3N4 nanosheets and MnO2 nanosheets, wherein the photoinduced electrons in MnO2 combined with the holes in g-C3N4, leading to enhanced charge carrier extraction and ut...

490 citations


Journal ArticleDOI
TL;DR: In this paper, a ternary Ag2CrO4/g-C3N4/GO composite photocatalyst was fabricated for photocatalytic CO2 reduction into methanol (CH3OH) and methane (CH4).
Abstract: Graphitic carbon nitride (g-C3N4)-based photocatalysts holds great promise on photocatalytic CO2 conversion into solar fules; however, the efficiency of pristine g-C3N4 is currently limited by its poor visible light absorption and rapid charge recombination. Employing silver chromate (Ag2CrO4) nanoparticles as photosensitizer and graphene oxide (GO) as cocatalyst, a novel ternary Ag2CrO4/g-C3N4/GO composite photocatalyst was fabricated for photocatalytic CO2 reduction into methanol (CH3OH) and methane (CH4). The ternary composites exhibited an enhanced CO2 conversion activity with a turnover frequency of 0.30 h–1, which was 2.3 times that of pristine g-C3N4 under simulated sunlight irradiation. The enhanced photocatalytic activity was due to broadened light absorption, higher CO2 adsorption and more efficient charge separation. Specifically, due to the matched band structure and appropriate loading ratio of Ag2CrO4, a direct Z-scheme Ag2CrO4/g-C3N4 heterojunction is formed, driven by the internal electric field across the Ag2CrO4/g-C3N4 interface. The formation of the direct Z-scheme heterojunction is substantiated by radical scavenging experiments and density functional theory calculations, and it benefits the photocatalytic reaction by accelerating the charge separation and improving the redox ability. Furthermore, GO cocatalyst not only promotes the charge transfer but also provides plentiful CO2 adsorption and catalytic sites. This work exemplifies the facile development of ternary g-C3N4-based photocatalysts with high CO2-conversion activity by coupling a small amount of Ag-based photosensitizer and metal-free cocatalyst.

440 citations


Journal ArticleDOI
20 Aug 2018
TL;DR: Recent topics in nanoscale Bi-based photocatalysts, including doping, changing stoichiometry, solid solutions, ultrathin nanosheets, hierarchical and hollow architectures, conventional heterojunctions, direct Z-scheme junctions, and surface modification of conductive materials and semiconductors, are reviewed.
Abstract: Nanoscale Bi-based photocatalysts are promising candidates for visible-light-driven photocatalytic environmental remediation and energy conversion. However, the performance of bulk bismuthal semiconductors is unsatisfactory. Increasing efforts have been focused on enhancing the performance of this photocatalyst family. Many studies have reported on component adjustment, morphology control, heterojunction construction, and surface modification. Herein, recent topics in these fields, including doping, changing stoichiometry, solid solutions, ultrathin nanosheets, hierarchical and hollow architectures, conventional heterojunctions, direct Z-scheme junctions, and surface modification of conductive materials and semiconductors, are reviewed. The progress in the enhancement mechanism involving light absorption, band structure tailoring, and separation and utilization of excited carriers, is also introduced. The challenges and tendencies in the studies of nanoscale Bi-based photocatalysts are discussed and summarized.

396 citations



Journal ArticleDOI
TL;DR: In this paper, a novel hybrid TiO2 nanofiber coated by CuInS2 nanoplates through a hydrothermal method was fabricated for CO2 reduction under irradiation.
Abstract: Photocatalytic CO2 reduction into solar fuels over photocatalysts has theoretically and practically become a hot research topic. Herein, we fabricated a novel hybrid TiO2 nanofiber coated by CuInS2 nanoplates through a hydrothermal method. The materials were characterized by X-ray diffraction, electron microscopes, UV–vis absorption spectra, nitrogen sorption, X-ray photoelectron spectroscopy and electrochemical impudence spectroscopy. The resulting TiO2/CuInS2 hybrid nanofibers exhibit superior photocatalytic activity for CO2 reduction under irradiation, due to the generation of direct Z-scheme heterojunction between TiO2 and CuInS2. This work may provide an alternate methodology to design and fabricate multicomponent TiO2-based photocatalyst for high-efficiency CO2 photoreduction.

365 citations


Journal ArticleDOI
01 Mar 2018-Small
TL;DR: The unique hierarchical Co3 O4 /NHCS core-shell structure with hierarchical structures is a promising electrode material for high-performance supercapacitors.
Abstract: Co3 O4 /nitrogen-doped carbon hollow spheres (Co3 O4 /NHCSs) with hierarchical structures are synthesized by virtue of a hydrothermal method and subsequent calcination treatment. NHCSs, as a hard template, can aid the generation of Co3 O4 nanosheets on its surface; while SiO2 spheres, as a sacrificed-template, can be dissolved in the process. The prepared Co3 O4 /NHCS composites are investigated as the electrode active material. This composite exhibits an enhanced performance than Co3 O4 itself. A higher specific capacitance of 581 F g-1 at 1 A g-1 and a higher rate performance of 91.6% retention at 20 A g-1 are achieved, better than Co3 O4 nanorods (318 F g-1 at 1 A g-1 and 67.1% retention at 20 A g-1 ). In addition, the composite is employed as a positive electrode to fabricate an asymmetric supercapacitor. The device can deliver a high energy density of 34.5 Wh kg-1 at the power density of 753 W kg-1 and display a desirable cycling stability. All of these attractive results make the unique hierarchical Co3 O4 /NHCS core-shell structure a promising electrode material for high-performance supercapacitors.

Journal ArticleDOI
TL;DR: In this paper, the first-principle calculation based on density functional theory is an effective approach to investigate the structural, electronic, optical and thermodynamic properties of molecules and crystals, which provides important information to elucidate the improved photocatalytic activity of modified g-C3N4 at atomic or unit-cell levels.
Abstract: Graphitic carbon nitride (g-C3N4) is an attractive photocatalyst which has appealing visible light absorption, outstanding layered porous structure, high stability and nontoxicity. Many experimental methods have been developed to modify the pristine g-C3N4 and enhanced photocatalytic activities have been witnessed. First-principle calculation based on density functional theory is an effective approach to investigate the structural, electronic, optical and thermodynamic properties of molecules and crystals, which provides important information to elucidate the improved photocatalytic activity of modified g-C3N4 at atomic or unit-cell levels, or even further, to predict the property and photocatalytic activity of experimentally un-synthesized g-C3N4-based photocatalysts. This review is dedicated to this important material, i.e. tri-s-triazine-based g-C3N4 and summarized a panorama of the major advances in the first-principle investigation. The existing challenges and future directions at the forefront of this emerging research hotpot have also been discussed.

Journal ArticleDOI
TL;DR: In this article, an electrostatic self-assembly method was exploited to prepare g-C3N4/ZnO composite microsphere, achieving a hierarchical structure with intimate contact between them.

Journal ArticleDOI
TL;DR: In this paper, hollow cobalt sulfide (CoS) is used as a cocatalyst to realize highly efficient photocatalytic hydrogen (H2) production in the field of solar energy conversion.
Abstract: Seeking for a suitable cocatalyst to realize highly efficient photocatalytic hydrogen (H2) production is a great challenge in the field of solar energy conversion. Herein, hollow cobalt sulfide (Co...

Journal ArticleDOI
03 Dec 2018-ACS Nano
TL;DR: In situ and in-depth observation of structural evolution in the OER measurement can provide insights into the fundamental understanding of the mechanism for the O ER catalysts, thus enabling the more rational design of low-cost and high-efficient electrocatalysts for water splitting.
Abstract: As one of the most remarkable oxygen evolution reaction (OER) electrocatalysts, metal chalcogenides have been intensively reported during the past few decades because of their high OER activities. It has been reported that electron-chemical conversion of metal chalcogenides into oxides/hydroxides would take place after the OER. However, the transition mechanism of such unstable structures, as well as the real active sites and catalytic activity during the OER for these electrocatalysts, has not been understood yet; therefore a direct observation for the electrocatalytic water oxidation process, especially at nano or even angstrom scale, is urgently needed. In this research, by employing advanced Cs-corrected transmission electron microscopy (TEM), a step by step oxidational evolution of amorphous electrocatalyst CoS x into crystallized CoOOH in the OER has been in situ captured: irreversible conversion of CoS x to crystallized CoOOH is initiated on the surface of the electrocatalysts with a morphology change via Co(OH)2 intermediate during the OER measurement, where CoOOH is confirmed as the real active species. Besides, this transition process has also been confirmed by multiple applications of X-ray photoelectron spectroscopy (XPS), in situ Fourier-transform infrared spectroscopy (FTIR), and other ex situ technologies. Moreover, on the basis of this discovery, a high-efficiency electrocatalyst of a nitrogen-doped graphene foam (NGF) coated by CoS x has been explored through a thorough structure transformation of CoOOH. We believe this in situ and in-depth observation of structural evolution in the OER measurement can provide insights into the fundamental understanding of the mechanism for the OER catalysts, thus enabling the more rational design of low-cost and high-efficient electrocatalysts for water splitting.


Journal ArticleDOI
TL;DR: This work underscores the tuned structure and electrocatalytic OER performance of MOF derivatives by the versatility of MXenes and provides insight into the structure-activity relationship for noble metal-free catalysts.
Abstract: Water oxidation is the key process for many sustainable energy technologies containing artificial photosynthesis and metal–air batteries. Engineering inexpensive yet active electrocatalysts for water oxidation is mandatory for the cost-effective generation of solar fuels. Herein, we propose a novel hierarchical porous Ni–Co-mixed metal sulfide (denoted as NiCoS) on Ti3C2Tx MXene via a metal–organic framework (MOF)-based approach. Benefiting from the unique structure and strong interfacial interaction between NiCoS and Ti3C2Tx sheets, the hybrid guarantees an enhanced active surface area with prominent charge-transfer conductivity and thus a superior activity toward oxygen evolution reactions (OERs). Impressively, the hierarchical NiCoS in the hybrid is converted to nickel/cobalt oxyhydroxide–NiCoS assembly (denoted as NiCoOOH–NiCoS) by OER measurement, where NiCoOOH on the surface is confirmed as the intrinsic active species for the consequent water oxidation. The hybrid material is further applied to an ...

Journal ArticleDOI
TL;DR: In this paper, a novel TiO2/NiS core-shell nanohybrid was fabricated where few-layer NiS nodes were used for photocatalytic water splitting to generate hydrogen.
Abstract: Photocatalytic water splitting to generate hydrogen (H2) is a sustainable approach for solving the current energy crisis. A novel TiO2/NiS core–shell nanohybrid was fabricated where few-layer NiS n...

Journal ArticleDOI
TL;DR: In this paper, Ni(OH) 2 has been used as a cocatalyst for photocatalytic hydrogen evolution and can also be used to enhance the photoreduction of CO2 into chemical fuels.
Abstract: In the past few years, Ni(OH)2 has been found to be an effective cocatalyst for photocatalytic hydrogen evolution. Herein, we report that it can also be used to enhance the photoreduction of CO2 into chemical fuels. Vertically aligned Ni(OH) 2 nanosheets are deposited onto electrospinning TiO2 nanofibers via simple wet-chemical precipitation to manufacture TiO2/Ni(OH) 2 hybrid photocatalysts. The TiO2 nanofibers can direct the ordered growth of Ni(OH) 2 nanosheets, which have a thickness of 20 nm and uniformly cover the surface of the TiO2 substrate. The TiO2/Ni(OH) 2 hierarchical composite displays remarkably improved photocatalytic CO2 reduction activity compared to that displayed by pristine TiO2 fibers. The bare TiO2 can only produce methane and carbon monoxide (1.13 and 0.76 μmol h−1 g−1, respectively) upon CO2 photoreduction. After loading 0.5 wt% Ni(OH) 2, the methane yield increases to 2.20 μmol h−1 g−1, meanwhile the CO yield is unchanged. Interestingly, alcohols (methanol and ethanol) also appear as products, in addition to CH4 and CO, over the TiO2/Ni(OH) 2 hybrid, and the maximum yield is reached with 15 wt% Ni(OH) 2 loading (0.58 and 0.37 μmol h−1 g−1 for methanol and ethanol, respectively). This can be ascribed to an enhanced charge separation efficiency and higher CO2 capture capacity due to the presence of Ni(OH) 2. These results demonstrate that Ni(OH) 2 can not only improve the total CO2 conversion efficiency, but can also alter the product selectivity upon photocatalysis. This work opens a new pathway for achieving high-efficiency photocatalytic CO2 reduction with Ni(OH) 2 as a cocatalyst.

Journal ArticleDOI
TL;DR: In this article, a hierarchical treated rape pollen (TRP) was used as a metal-free catalyst for visible-light-driven photocatalytic CO2 reduction, achieving a high quantum efficiency of over 6.7% at 420 nm.
Abstract: We demonstrate a rational fabrication of hierarchical treated rape pollen (TRP), a biological material used as a metal-free catalyst for visible-light-driven photocatalytic CO2 reduction. The TRP catalyst exhibits excellent visible-light-driven carbon monoxide (CO) formation of 488.4 μmol h−1 g−1 with 98.3% selectivity, using no co-catalyst or sacrifice reagent, accompanied by a high quantum efficiency of over 6.7% at 420 nm. The CO evolution rate obtained on the TRP catalyst is roughly 29.4 and 25.6 times higher than those of the most commonly reported photocatalysts, such as g-C3N4 (16.6 μmol h−1 g−1) and P25 TiO2 (19.1 μmol h−1 g−1), and is the highest among the reported carbon-based photocatalysts. In situ Fourier transform infrared spectrometry analysis disclosed that formic acid is a major intermediate. The considerable photocatalytic CO2 reduction activity observed on the TRP catalyst can be ascribed to the following factors: (i) the unique hollow porous structure of the TRP favours visible light harvesting and CO2 adsorption capacity; and (ii) the interior cavity of the TRP can decrease the diffusion length of the photogenerated reactive charge carrier from bulk to surface, thus promoting charge carrier separation. We anticipate that such a nature-based sustainable photocatalyst can provide new insights to facilitate the design of metal-free catalysts with outstanding visible-light-driven CO2 reduction performance.

Journal ArticleDOI
TL;DR: In this paper, a series of g-C3N4/polydopamine composites were successfully fabricated by in situ polymerization of dopamine on the surface of the composite.
Abstract: Photocatalytic water splitting is a promising strategy to convert solar energy into chemical energy. Herein, a series of g-C3N4/polydopamine (g-C3N4/PDA) composites were successfully fabricated by in situ polymerization of dopamine on the g-C3N4 surface. Among all the as-prepared composites, the best photocatalytic hydrogen evolution rate of the as-prepared composites was up to 69 μmol h–1 under the irradiation of visible light (λ > 420 nm), which was about 4.5 times than that of pristine g-C3N4 (16 μmol h–1). The enhancement of photocatalytic H2 evolution is reasonably attributed to the markedly enhanced light harvesting, broadened spectral response range and low onset potential of H2 production, as well as effective separation and rapid transportation of photogenerated charge carriers. More importantly, the surface modification of g-C3N4 by a small amount of PDA can effectively inhibit the overgrowth of Pt nanoparticles (NPs) during the photocatalytic reactions, which promotes the photoelectron injectio...

Journal ArticleDOI
TL;DR: In this paper, a novel 1D/2D TiO2/MoS2 nanostructured hybrid with 2D transition metal dichalcogenides was fabricated for photoreduction of CO2.
Abstract: Photocatalytic reduction of CO2 into solar fuels is recognized an attractive approach to solve the environmental and energy crisis. MoS2, a type of 2D transition metal dichalcogenides, has attracted significant attention in photoelectronics, sensors and photo/electrocatalytic water splitting owing to its remarkable properties. Nevertheless, to date, MoS2 is barely used as (co)catalyst for CO2 photoreduction. Herein, novel 1D/2D TiO2/MoS2 nanostructured hybrid with TiO2 fibers covered by MoS2 nanosheets by hydrothermal transformation method is fabricated. The MoS2 sheet arrays show a lateral size of ≈80 nm and a thickness of down to 2 nm, vertically and uniformly standing upon the TiO2 fibers. X‐ray photoelectron spectroscopy (XPS) results and density functional theory (DFT) calculation imply the intimate chemical interaction between MoS2 and TiO2 upon hybridization, which can facilitate electron–hole separation upon photoexcitation. In addition, the hierarchical TiO2/MoS2 nanostructure shows enhanced optical absorption and CO2 adsorption, therefore, a superior photocatalytic activity for reducing CO2 into methane and methanol is achieved over the hybrid as compared to pristine TiO2. Isotope (13C) tracer test confirms that the products are produced from the photocatalytic reduction of the CO2 source instead of any organic contaminants. This work offers an alternative approach to rationally design and synthesize TiO2‐based photocatalysts toward high‐efficiency photoreduction of CO2.

Journal ArticleDOI
Tong Tong1, Bicheng Zhu1, Chuanjia Jiang1, Bei Cheng1, Jiaguo Yu1 
TL;DR: In this article, the structural, electronic and optical properties of single-atom Pt, Pd and Au loaded on bilayer graphitic carbon nitride (g-C 3 N 4 ) substrate were investigated by density functional theory (DFT) simulations.

Journal ArticleDOI
TL;DR: In this paper, the fundamental principles on the photocatalytic pollutant degradation were systematically introduced, and the important considerations in the design of photocatalyst degradation systems were carefully addressed, including charge carrier dynamics, catalytic selectivity, photocat catalyst stability, pollutant adsorption and photodegradation kinetics.
Abstract: Heterogeneous photocatalysis has long been considered to be one of the most promising approaches to tackling the myriad environmental issues However, there are still many challenges for designing efficient and cost-effective photocatalysts and photocatalytic degradation systems for application in practical environmental remediation In this review, we first systematically introduced the fundamental principles on the photocatalytic pollutant degradation Then, the important considerations in the design of photocatalytic degradation systems are carefully addressed, including charge carrier dynamics, catalytic selectivity, photocatalyst stability, pollutant adsorption and photodegradation kinetics Especially, the underlying mechanisms are thoroughly reviewed, including investigation of oxygen reduction properties and identification of reactive oxygen species and key intermediates This review in environmental photocatalysis may inspire exciting new directions and methods for designing, fabricating and evaluating photocatalytic degradation systems for better environmental remediation and possibly other relevant fields, such as photocatalytic disinfection, water oxidation, and selective organic transformations

Journal ArticleDOI
TL;DR: In this article, the authors found that the order of adding TEOA into the reaction system before or after the photodeposition of Pt had a significant effect on photocatalytic hydrogen production over graphitic carbon nitride nanosheets.
Abstract: Photocatalytic H2 production plays an important role in alleviating fossil fuel crisis and constructing a sustainable world. Graphitic carbon nitride nanosheets (CNS), coupled with cocatalyst platinum (Pt) and hole sacrificial agent triethanolamine (TEOA), often show excellent H2-production activity. However, the question on maximizing Pt amount in this given TEOA-contained system still remains unsolved. Herein, it was found that the order of adding TEOA into the reaction system before or after the photodeposition of Pt had a significant effect on photocatalytic hydrogen production over CNS. Specifically, the content of Pt was lower when TEOA was added beforehand, implying that a strong interaction existed between the Pt-precursor H2PtCl6 and TEOA, thus curbing the photoreduction to metallic Pt. Therefore, a roughly 4-fold increment in hydrogen production activity (4210.8 vs. 972.2 μmol h–1 g–1) was obtained by merely swapping the sequence of the addition of TEOA. Moreover, the apparent quantum efficiency...

Journal ArticleDOI
TL;DR: In this article, the metal-organic framework-8 (ZIF-8) is applied to demonstrate the first MOF-based surface passivation layer in a PEC water-splitting system.
Abstract: DOI: 10.1002/aenm.201800101 Among them, ZnO is considered as one of the most promising candidates, owing to its low cost, nontoxicity, direct bandgap, and excellent electron mobility.[5] Nevertheless, the limited hole mobility and slow kinetics at the ZnO/electrolyte interface usually results in a rather low charge separation and transfer efficiency. Besides, the durability of ZnO-based photoelectrodes is typically limited by photoinduced corrosion. To tackle the aforementioned drawbacks, a variety of strategies have been developed, mainly based on architecture engineering and surface modification.[7] The high surface-to-volume ratio, short lateral charge transport length, and low light reflectivity associated with 1D ZnO nanoarchitectures give rise to higher photoconversion efficiency, compared to the bulk counterparts.[7] However, the presence of diverse surface states, such as oxygen vacancies, results in severe charge recombination. In this regard, surface passivation is highly recommended, because surface state passivation with suitable coatings, such as amorphous TiO2, Al2O3, etc., was demonstrated as an efficient way to decrease the trap statemediated charge recombination.[4a,5b,6c,8] Moreover, the surface passivation layer also helps to prevent photocorrosion.[4a] Nevertheless, most of surface passivation layers rely on expensive and time-consuming atomic layer deposition routes. Besides, the coating transparency and the interfacial adhesion are usually poor. Therefore, exploring novel coating materials and facile fabrication procedures for alternative surface passivation layers is still highly challenging. Metal-organic frameworks (MOFs), as a novel class of porous materials built from metal clusters and organic ligands, have exhibited widespread applications because of their high porosity and surface functionalization.[9] However, to our knowledge, the use of MOFs in PEC systems has been poorly investigated. In this study, ZIF-8 is applied to demonstrate the first MOFbased surface passivation layer in a PEC water-splitting system. ZIF-8 is chosen thanks to its excellent transparency in the UV– visible range and good affinity with ZnO moieties. Uniform ZIF-8 layer with controllable thickness can be grown on the ZnO surface, forming a core–shell structure, by a simple solvothermal assisted in situ interfacial reaction.[10] The ZIF-8 overlayer not only helps to passivate surface states, but also protects the underlying ZnO from photocorrosion. As a consequence, the ZIF-8 passivated ZnO nanorod arrays (NRARs) exhibit a This study introduces zeolitic imidazolate framework-8 (ZIF-8) as the first metal-organic framework based transparent surface passivation layer for photo-electrochemical (PEC) water splitting. A significant enhancement for PEC water oxidation is demonstrated based on the in situ seamless coating of ZIF-8 surface passivation layer on Ni foam (NF) supported ZnO nanorod arrays photoanode. The PEC performance is improved by optimizing the ZIF-8 thickness and by grafting Ni(OH)2 nanosheets as synergetic co-catalyst. With respect to ZnO/NF, the optimized Ni(OH)2/ZIF-8/ZnO/NF photoanode exhibits a two times larger photocurrent density of 1.95 mA cm−2 and also a two times larger incident photon to current conversion efficiency of 40.05% (350 nm) at 1.23 V versus RHE (VRHE) under AM 1.5 G. The synergetic surface passivation and the co-catalyst modification contribute to prolonging the charge lifetime, to promoting the charge transfer, and to decreasing the overpotential for water oxidation.

Journal ArticleDOI
TL;DR: In this paper, hierarchical porous ZnO microspheres were synthesized by hydrothermal treatment of precursor zinc salts and subsequent low-temperature (300°C) calcination for 2.5h, and the photocatalytic properties of the as-prepared hexagonal wurtzite zinc oxide were examined by degrading Rhodamine B under simulated solar light.

Journal ArticleDOI
TL;DR: In this article, a flexible bio-inspired Zn 0.5 Cd0.5 S@PAN (polyacrylonitrile) mat-shaped photocatalyst with a leaf-like structure is presented.
Abstract: Photocatalytic hydrogen generation from water splitting offers a viable potential solution for utilizing solar energy. Here we report a feasible synthesis of flexible bio-inspired Zn 0.5 Cd 0.5 S@PAN (polyacrylonitrile) mat-shaped photocatalyst with leaf-like structure, which shows high photocatalytic H 2 -production activity with a rate of 475 μmol h −1 per 50 mg of the photocatalyst and an apparent quantum efficiency of 27.4% at 420 nm. The hierarchically porous structure of the mat-shaped Zn 0.5 Cd 0.5 S@PAN greatly enhances the molecular diffusion/transfer kinetics, and enlarges the utilization efficiency of light through the multiple reflections and scattering effect. Moreover, a good dispersion of Zn 0.5 Cd 0.5 S nanoparticles (NPs) on the surface of PAN nanofibers prevents their aggregation. These features account for high H 2 -production activity of Zn 0.5 Cd 0.5 S@PAN. Remarkably, the integrity and flexibility of Zn 0.5 Cd 0.5 S@PAN mat-shaped photocatalyst facilitate their separation and re-use after photocatalytic reaction. Hierarchically porous leaf-like mat-shaped photocatalysts with high photocatalytic activity and stability should also find potential applications in solar cells, catalysis, separation and purification processes.

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TL;DR: NiO/C-HS, with well-dispersed NiO nanosheets supported by carbon hollow spheres, exhibited excellent electrochemical performance and was heuristic for the design of other composites and suitable for ameliorating the poor stability of transition metal oxides.

Journal ArticleDOI
TL;DR: In this paper, the authors immobilize BP quantum dots (BPQDs) onto graphitic carbon nitride (g-C3N4) nanosheets to create a 0D-2D inorganic-organic hybrid via a conventional and cost-effective sonication approach.