APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
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IF 22.1
Sijia Liu,Xifei Zhou,Changqing Yang,Chaohai Wei,Yun Hu
The extensive use of sacrificial agents and the low carrier separation and utilization efficiency remain important factors limiting the development of photocatalytic hydrogen production . We report a three-layered, dual-functional photocatalysts of Cu atomics@UiO-66-NH 2 (U6N)/ZnIn 2 S 4 nanosheets (ZIS), for the simultaneous production of photocatalytic hydrogen and degradation of organic pollutants . When common and highly toxic organic pollutants (phenolic compounds and antibiotics) were substituted for the sacrificial agents, Cu@U6N/ZIS exhibited superior sustained hydrogen production, approximately 28 times greater than that of pure ZIS. The experimental results suggested that the window size of U6N (< organic pollutants molecular size) separates the reaction sites of organic pollutants oxidation and reduction of hydrogen ions (H + ), thereby achieving spatial separation of redox sites. Besides, the structure of Cu@U6N/ZIS, which was anchored Cu within U6N and encapsulated by ZIS nanosheets, forming Z-type heterojunctions, achieved the control of the directional transfer of photogenerated electrons. And the coupled system can effectively enhance water quality by reducing the biological toxicity of the wastewater. This study suggests new avenues for environmental restoration and non-fossil fuel production.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2018
·
IF 11.698
Tingting Hou,Nengchao Luo,Yi-Tao Cui,Jianmin Lu,Lei Li,Katherine E. MacArthur,Marc Heggen,Ruotian Chen,Fengtao Fan,Wenming Tian,Shengye Jin,Feng Wang
Engineering the electronic properties of heterogeneous catalysts is an important strategy to enhance their activity towards CO 2 reduction. Herein, we prepared partially sulfurized cerium oxide (CeO x -S) nanoclusters with the size less than 2 nm on the surface of ZnIn 2 S 4 layers. Surface electronic properties of CeO x -S nanoclusters are facilely modulated by cerium coordination to sulfur, inducing the emergence of abundant Ce 3+ and oxygen vacancies. For the photoreduction of CO 2 , CeO x -S/ZnIn 2 S 4 hybrid catalysts exhibited a CO productivity of 1.8 mmol g −1 with a rate of 0.18 mmol g −1 h −1 , which was twice as higher as that of ZnIn 2 S 4 catalyst using triethylamine as a sacrificial electron donor. Further mechanistic studies reveal that the photogenerated electrons are trapped by oxygen vacancies on CeO x -S/ZnIn 2 S 4 catalysts and subsequently transfer to CO 2 , benefiting the activation of CO 2 . Moreover, the extremely high selectivity of CO is derived from the weak adsorption of CO on the surface of CeO x -S/ZnIn 2 S 4 catalysts.
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CHEMOSPHERE
·
2022
·
IF 8.943
Jianhua Yang,Lu Fang,Zhengkui Li,Guanhua Meng,Yong Jia,Yongbin Jiang,Jianjun Lian,Xinhong Gan
At present, the researches on photocatalysis were mainly focused on the design, improvement and development of catalysts, and less attention was paid to the existing characteristics of environmentally persistent free radicals (EPFRs) during the process of photocatalytic oxidation. In this study, A flower-like Z-type heterojunction ZnO/ZnIn 2 S 4 (ZnO/ZIS) and typical antibiotic ceftriaxone sodium (CS) were taken as study objects, concentrating on the generation characteristics of EPFRs during the degradation of CS by ZnO/ZIS, and clarifying the degradation mechanism of CS in which EPFRs participated. The results showed that the degradation efficiency of 10 mg/L CS by 0.40 g/L ZnO/ZIS reached 85.3% in 150 min under the irradiation of 500 W xenon lamp . It was clear that ·O 2 − and h + play major roles in CS degradation by ZnO/ZIS under visible light, and ·OH plays an auxiliary role. Furthermore, the formation mechanism of EPFRs during photocatalytic degradation processes of CS by ZnO/ZIS were first investigated thoroughly via experimental analysis and density functional theory (DFT) calculations. The concentration level of EPFRs centered on oxygen atoms is 10 11 spin/mm 3 , which were generated in the process of degradation of CS by ZnO/ZIS under visible light. The production of EPFRs chiefly includes two procedures: chemical adsorption and transfer of electrons. The adsorption energy of precursor P8 on ZnIn 2 S 4 side is −1.91 eV, the electrons transferred from precursor P8 and P11 to ZnO/ZnIn 2 S 4 heterojunction. Surprisingly, EPFRs have little negative effects on the degradation process of CS by ZnO/ZIS. The study was not only a key field in the development of photocatalysis technology , but also a new way to study the removal mechanism of antibiotics.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Fangshu Xing,Renyou Zeng,Chuchu Cheng,Qiuwen Liu,Caijin Huang
Efficient aromatic alcohol oxidation with simultaneous H 2 evolution under aqueous conditions is achieved in a polyoxometalate (POM)-incorporated ZnIn 2 S 4 dual-functional photocatalytic system. The synergy between HPM and ZIS contributes to the formation of a Z-type heterojunction structure and thus enhances redox capacity. Moreover, the sub-nanometer size of POM clusters endows molecular-level interfacial contact, which acts as an "electron bridge" ensuring faster interfacial charge transfer kinetics. Therefore, an impressive nearly 100% yield of benzaldehyde and 10.6 mmol·g −1 ·h −1 H 2 -evolution rate are observed for POM/ZIS nanocomposites even under an anaerobic atmosphere with water as the solvent. This is the first application of POM-based materials in the anaerobic oxidation of benzyl alcohol with concomitant H 2 production. This study expands the possibilities for designing multifunctional POM-based photocatalysts for economic and ecological photoredox applications.
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Materials Chemistry Frontiers
·
2022
·Vol. 6
·期 13
·1795-1802
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IF 8.683
Bojing Sun,Dingge Fan,Xiaoyu Chen,Zhenzi Li,Wei Zhou,Yuncehn Du
Visible-light-driven photocatalytic overall pure water splitting is still a challenge, especially with single-component photocatalysts. Herein, ultrathin ZnIn2S4 nanosheets with Al doping (Al-ZIS) were fabricated via a one-step solvothermal method with magnetic stirring and could realize stoichiometric H2 and O2 evolution in pure water. The introduction of Al atoms not only adjusted the electronic configuration and improved the carrier density of atomic layers but also accelerated the separation efficiency of photogenerated charge carriers due to the formation of a domain electrostatic potential difference. Moreover, the positive charge enriched Al atoms are favorable for the adsorption of H2O molecules, which greatly boost the oxygen evolution reaction (OER) process on the Al-ZIS nanosheets. As a result, the photocatalysts achieved average H2 and O2 evolution rates of 77.2 and 35.3 μmol g−1 h−1, respectively, under visible-light irradiation and an apparent quantum yield (AQE) of 1.61% at 420 nm. This study provides new insights for introducing a heteroatom strategy to prepare other high-performance single-component photocatalysts for overall water splitting.
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CHEMICAL ENGINEERING JOURNAL
·
2022
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IF 16.744
Junhao Huang,Qingyong Tian,Huajian Feng,Chao Xue,Jun Li,Qun Xu
Construction of photocatalysts with efficient light-harvesting and charge separation properties for boosting photocatalytic hydrogen (H 2 ) evolution is still a challenge. Herein, a three-dimensional (3D) porous WS 2 @C@ZnIn 2 S 4 skeleton heterojunction is successfully synthesized by epitaxial growth of ZnIn 2 S 4 nanosheets on the WS 2 @C skeleton. The optimal WS 2 @C@ZnIn 2 S 4 photocatalyst exhibits considerable photocatalytic H 2 evolution rate (11.15 mmol·g −1 ·h −1 ) and CO 2 -to-CH 4 production performance (43.29 μmol·g −1 ), respectively. The high photocatalytic performance can be ascribed to the fact that multiple light reflection and scattering behaviors originated from 3D architecture facilitates to prolong the interaction length between photons and catalyst, which significantly enlarging the light-harvesting ability and utilization efficiency. Importantly, highly conductive WS 2 @C skeleton can drive photo-induced charge transportation from ZnIn 2 S 4 to WS 2 co-catalyst via the interfacial charge-transfer pathways. The DFT calculations further demonstrate the promotional effects of multiple diffuse reflection and separation of photo-generated carriers in photocatalytic H 2 evolution.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2022
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IF 6.371
Qiang Gao,Junxi Li,Bin Liu,Chenguang Liu
The rationally designed semiconductor photocatalytic materials have attracted significant attention because of their huge advantages in the use of solar light. Herein, a series of direct Z-scheme heterojunction nanocomposites were synthesized via in situ growth of zinc indium sulfide nanosheets on ceria nanosheets (ZnIn 2 S 4 @CeO 2 ) and employed for effective photodegradation and Cr(VI) reduction. Advanced characterizations such as XPS , EPR spectra, and DFT calculations verified that the formation of direct Z-scheme charges transfer mechanism promoted rapid charge separation and retained strong redox capacity. As a result, the optimized ZnIn 2 S 4 @CeO 2 sample showed significantly promoted photocatalytic removal rates for tetracycline (TC) and Cr(VI) at a 3.7 and 4.5 times enhancement by comparison with the pristine ZnIn 2 S 4 , respectively. Additionally, after four consecutive cyclic tests, the as-synthesized nanocomposite exhibited remarkable photocatalytic activity and stability. The present work provides an integrated engineering strategy for Z-scheme photocatalyst systems with high photocatalytic efficiency and extensive applications.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Lin Liu,Jiaqing Liu,Weijie Yang,Jun Wan,Feng Fu,Danjun Wang
Energy band structures greatly determine the charge separation and transfer properties in heterojunction photocatalysts and consequently their photocatalytic activities. Herein, a well-designed Z-scheme ZnIn 2 S 4 -S/CNTs/RP (ZIS-S/CNTs/RP) nanocomposite was fabricated according to an energy band alignment steering strategy to realize superior photocatalytic H 2 evolution performance. The ZIS-S/CNTs/RP nanocomposite shows an efficient photocatalytic H 2 evolution rate of 1639.9 μmol g -1 h −1 , which is noticeably higher than that of pristine red phosphorus (RP) and CNTs/RP and ZIS-S/RP composites, as well as those of the compared heterojunctions using bulk RP or ZnIn 2 S 4 . Owing to the modification of nanosized RP and the introduction of sulfur vacancies in ZnIn 2 S 4 , a tailored energy band alignment of the heterojunction with a higher reduction potential and larger Fermi level potential difference was achieved, which resulted in significantly increased photogenerated electron-hole separation efficiency and a more efficient Z-scheme charge transfer mechanism, thus promoting the photocatalytic activity of ZIS-S/CNTs/RP. This work aims to provide a novel effective strategy for the construction of high-performance heterojunction photocatalysts by energy band engineering.
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Science China-Chemistry
·
2021
·Vol. 64
·期 10
·1716-1722
·
IF 9.445
Chao Yuguang,Zhang Weiyu,Zhou Peng,Chen Hui,Lu Shiyu,Li Menggang,Zhang Qinghua,Gu Lin,Guo Shaojun
Atomic sites co-catalyst (ASC) on photocatalytic materials possesses an attractive prospect to promote charge carrier separation and tune surface reaction kinetics, yet the synthesis of earth-abundant ASC under low temperature remains a great challenge. Here, a novel in-situ NH 4 + -etched strategy to anchor atomic Mo sites on ZnIn 2 S 4 hierarchical nanotubes (HNTs) with abundant mesopores under mild conditions for promoting charge carrier separation and enhancing light multi-reflections is developed for efficient photocatalytic H 2 evolution. Density functional theory calculations and linear sweep voltammetry demonstrate that the well-defined Mo-S 2 O 1 sites with distinctive coordination configuration and electronic property contribute to the enhanced separation of photo-generated charge carriers and reduced Gibbs free energy for H 2 evolution. Consequently, the well-defined MoSA-ZIS HNTs present an excellent photocatalytic activity with a rate of 29.9 µmol h −1 (5.98 mmol g −1 h −1 ), which is 7.3 times higher than that of ZnIn 2 S 4 nanosheets (NSs), to be among the best ZnIn 2 S 4 -based photocatalysts. The present strategy breaks the high-temperature limitation of conventional top-down thermal dissociation/emitting approach for anchoring non-noble metal atomic sites on catalyst support.
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MICROCHIMICA ACTA
·
2024
·Vol. 191
·期 5
·1-12
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IF 5.3
Zhou Yu,Xiao Wei,Tian Gang,Zhang Suni,Wei Xiaoping,Li Jianping
A novel ternary heterojunction material In 2 O 3 /In 2 S 3 /ZnIn 2 S 4 was synthesized, and a photoelectrochemical sensor was fabricated for the non-invasive test of dopamine (DA) in sweat. In 2 O 3 multihollow microtubules were synthesized and then In 2 S 3 was formed on their surface to construct a type-I heterojunction between In 2 S 3 and In 2 O 3 . ZnIn 2 S 4 was further introduced to form a Z-scheme heterojunction between In 2 S 3 /ZnIn 2 S 4 . Under photoexcitation, the photogenerated holes of In 2 O 3 transferred to the valence band of In 2 S 3 , superimposed with the holes produced by In 2 S 3 , leads to a significantly higher photocatalytic oxidation capacity of In 2 O 3 /In 2 S 3 /ZnIn 2 S 4 ternary composites than that of In 2 O 3 /In 2 S 3 . The Z-scheme heterojunction accelerates the transfer of photogenerated electrons accumulated on the type-I heterojunction. In the presence of DA, it is rapidly oxidized into polydopamine (PDA) by In 2 O 3 /In 2 S 3 , and the benzoquinone groups of PDA compete for the photogenerated electrons to reduce the current in the external circuit, whereby DA determination is achieved. Owing to the combination of type-I and Z-scheme heterojunction, the sensor showed extremely high sensitivity, with a detection limit of 3.94 × 10 −12 mol/L. It is one of the most sensitive methods for DA detection reported and has been applied to the determination of DA in human sweat. Graphical Abstract
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2024
·
IF 5.8
Zhuo Liu,Chao Xiong,Lin Gan,Junhui Yin,Xueying Wang,Jintao Li,Jiayi Wang,Jintong Li,Changyu Lu
In this work, the S-scheme MnFe 2 O 4 /ZnIn 2 S 4 (MFO/ZIS) heterostructure was prepared by hydrothermal method, which can degrade tetracycline (TC) and 2,4,6-trinitrotoluene (TNT) efficiently. Under simulated sunlight irradiation, 88.9 % of TC can be degraded within 75 minutes, and 82.7 % of TNT can be degraded within 120 minutes. The photocurrent response of 3 %MFO/ZIS (0.45 µA cm- 2 ) surpassed that of ZIS (0.15 µA cm −2 ) and MFO (0.08 µA cm −2 ). This is mainly due to the synergistic effect of the S-scheme electron transport pathway and the photothermal effect in MFO/ZIS, which improves its utilization rate of photogenerated electrons. After being used four times, 3 %MFO/ZIS can still degrade 80.2 % of TC, showing excellent stability. In addition, the TC degradation process was analyzed and the low toxicity of TC after degradation was confirmed by LC-MS, ECOSAR and experiments of cultivating mung bean sprouts, demonstrating the potential application value of MFO/ZIS heterojunction in the wastewater treatment field.
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FUEL
·
2024
·
IF 6.7
Yuzhou Xia,Jilong Xiao,Jiacheng Zhang,Renkun Huang,Xiaohui Huang,Guiyang Yan,Liuping Zheng
The construction of step-scheme (S-scheme) heterojunction has become an effective strategy for enhancing photocatalytic CO 2 reduction. In this study, a sunflower-like S-scheme WO 3 /ZnIn 2 S 4 heterostructure is fabricated through the in-situ growth of ZnIn 2 S 4 nanosheets on WO 3 hollow sphere, aimed at improving selective CO 2 reduction. The constructed embedding configuration, featuring a WO 3 hollow sphere core and an outer layer of ZnIn 2 S 4 nanosheet, increases the contact interface and establishes a significant built-in electric field, thereby promoting the migration and separation of photogenerated carriers. The confined internal cavity of the three-dimensional (3D) sunflower-like architecture aids in limiting the free diffusion of CO 2 , and enriching CO 2 molecules at the surface of the photocatalyst, consequently enhancing reaction kinetics. Moreover, S vacancies on ZnIn 2 S 4 nanosheets promote the chemisorption and activation of CO 2 . As a result, the optimized evolution rates for CH 4 and CO of 58.7μmol g –1 h −1 and 51.3μmol g –1 h −1 , respectively, are achieved for WO 3 /ZnIn 2 S 4 heterojunction. The corresponding electron selectivity for CH 4 reaches 82.1 %, which is 13 and 1.5 times higher than those of bare WO 3 and ZnIn 2 S 4 , respectively. This provides valuable insights into the design of muti-functionalized S-scheme heterojunction photocatalysts.
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