CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Zuming He,Kai Lin,Ngie Hing Wong,Jaka Sunarso,Yongmei Xia,Xiaofei Fu,Jiangbin Su,Zhengyi Huang,Yong Wang,Bin Tang
Semiconductor photocatalysis technology for environmental remediation faces primary challenges, such as charge-carrier recombination and interfacial charge transfer inhibition, which affect its degradation efficiency in removing organic contaminants. In this work, we successfully synthesized a unique Z-scheme KNbO 3 /ZnIn 2 S 4 hollow core–shell microsphere via a combined hard template, thermal treatment, and hydrothermal processes as the photocatalyst for ciprofloxacin (CIP), oxytetracycline hydrochloride (OTCH), and rhodamine B (RhB) remediation under sunlight irradiation. Compared to the pure KNbO 3 and ZnIn 2 S 4 , our optimized 15-KNbO 3 /ZnIn 2 S 4 composite exhibited enhanced photodegradation performance with up to 99.8 %, 96.8 % and 97.5 % for CIP, OTCH, and RhB removal within 110 min, respectively. At the KNbO 3 /ZnIn 2 S 4 heterojunction interface, the composite developed its internal electric field and enhanced its photoabsorption under visible light region, thus boosting its charge separation. Subsequently, we evaluate the removal of total organic carbon (TOC) concentration and the influence of different ions on CIP degradation. In addition, we systematically investigated the Z-scheme charge migration process within the heterojunction with a series of experiments. Our results indicated that the hydroxyl and superoxide radicals were the dominant active species during photocatalysis. The composite also could achieve excellent stability and adaptability. We also managed to identify the CIP-degraded intermediates and deduce their possible degradation pathways. Lastly, our toxicity analysis revealed that CIP toxicity could decrease gradually during photocatalysis. In this work, we presented a unique method for preparing inexpensive and highly efficient Z-scheme hollow core–shell structure photocatalysts with excellent antibiotic remediation in water under simulated sunlight illumination.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2021
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IF 8.128
Quan Zhang,Xiaohao Wang,Juhua Zhang,Lingfeng Li,Huajun Gu,Wei-Lin Dai
The directional synthesis of transition metal phosphides was considered to be an effective strategy to solve the overdependence of noble metals on photocatalytic hydrogen evolution (PHE) reactions. Inspiringly, this work reported a facile method for constructing hollow Co 2 P nanocages (Co 2 P NCGs) that derived from ZIF-67 by calcining and phosphiding procedure in nitrogen atmosphere to act as non-noble metal cocatalysts. Followed with further coating thin-layered ZnIn 2 S 4 (ZIS) on the surface of Co 2 P NCGs through a hydrothermal reaction , the hierarchical robust Co 2 P/ZnIn 2 S 4 nanocages (Co 2 P/ZIS NCGs) were then delicately fabricated as efficient photocatalysts for PHE reactions. The uniquely hollow structure of Co 2 P NCGs largely diffused the photogenerated chargers that induced from ZIS and the closely interfacial contact significantly promoted the separation and transfer of electrons from ZIS to Co 2 P according to density functional theory (DFT) calculation, synergistically resulting in an efficient hydrogen generation performance. PHE results showed that an efficient H 2 evolution rate of 7.93 mmol/g/h over 10% Co 2 P/ZIS NCGs was achieved, about 10 times higher than that of pristine ZnIn 2 S 4 . More importantly, the hierarchically hollow Co 2 P/ZIS NCGs exhibited ascendant PHE activity in comparison with that of 1% noble metal (Pt, Au, Ag) loaded ZnIn 2 S 4 with superior sustainability, all indicating the efficient and stable photocatalysts of Co 2 P/ZIS NCGs for PHE reactions.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2020
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IF 16.683
Yingying Qin,Hong Li,Jian Lu,Yonghai Feng,Fanying Meng,Changchang Ma,Yongsheng Yan,Minjia Meng
Fabricating 2D/2D heterojunction with vacancy is more favorable to the spatial separation and transfer of charge owing to the matching of unique 2D structure and vacancy engineering, but the regulation and observation of interlayer forces and electronic structure is a challenging task for synthesizing heterojunction photocatalyst and studying the photocatalytic hydrogen evolution mechanism. Herein, an original 2D/2D ZnIn 2 S 4 /g-C 3 N 4 Van der Waals heterojunction with S vacancies (ZIS-S/CN VDW) photocatalyst are firstly engineered. The optimized 30ZIS-S/g-C 3 N 4 has the highest H 2 evolution rate of 6095.1 μmol h −1 g −1 , which is primarily attributed to the fact that 2D/2D VDW heterojunction possesses larger contact area and strong electronic interaction to stimulate charge kinetics, and the vacancy engineering can enhance light absorption by regulating the electronic band structure and act as effective active sites for capturing electrons. This work not only enriches 2D/2D heterojunction photocatalytic system based on g-C 3 N 4 , but also provides alternative proposal for engineering 2D/2D heterojunction photocatalyst with satisfactory performance.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Jundie Hu,Tingyu Yang,Junjie Chen,Xiaogang Yang,Jiafu Qu,Yahui Cai
Hydrogen peroxide (H 2 O 2 ) is a significant green oxidant for environment and new energy, especially for Fenton-like system. Onsite production and sustainable consumption of H 2 O 2 are the two critical challenges. Here, a fantastic 2D/1D hierarchical layered ZnIn 2 S 4 /TiO 2 heterojunction is reported as an efficient catalyst for in- situ H 2 O 2 production via 2-electrons oxygen reduction (ORR) process and be rapidly activated to high concentration hydroxyl radical (•OH) for water purification under visible light irradiation. The high-quality catalyst enables superior H 2 O 2 production rate of 1530.59 μmol h −1 g −1 with an external quantum efficiency of 10.39% illuminated at 400 nm, is much higher than that of reported photocatalysts. The bimetallic sulfide ZnIn 2 S 4 can effectively promote the activation of H 2 O 2 due to the unsaturation of sulfur atoms, so that the wastewater containing tetracycline (50 ppm) can be degraded by 90% only within 60 min by ZnIn 2 S 4 /TiO 2 via this cascade reaction. This work provides a novel strategy and ZnIn 2 S 4 -based catalyst for photocatalytic Fenton-like reaction.
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Nanomaterials
·
2018
·Vol. 8
·期 7
·472
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IF 3.504
Siyu Xu,Jun Dai,Juan Yang,Jun You,Jingyi Hao
A series of novel and efficient heterostructured composites CaIn2S4/ZnIn2S4have been synthesized using a facile hydrothermal method. XRD patterns indicate the as-prepared catalysts are two-phase composites of cubic phase CaIn2S4and hexagonal phase ZnIn2S4. FESEM (field emission scanning electron microscope) images display that the synthesized composites are composed of flower-like microspheres with wide diameter distribution. UV–Vis diffuse reflectance spectra (DRS) show that the optical absorption edges of the CaIn2S4/ZnIn2S4composites shift toward longer wavelengths with the increase of the CaIn2S4component. The photocatalytic activities of the as-synthesized composites are investigated by using the aqueous-phase Cr(VI) reduction under simulated sunlight irradiation. This is the first report on the application of the CaIn2S4/ZnIn2S4composites as stable and efficient photocatalysts for the Cr(VI) reduction. The fabricated CaIn2S4/ZnIn2S4composites possess higher photocatalytic performance in comparison with pristine CaIn2S4or ZnIn2S4. The CaIn2S4/ZnIn2S4composite with a CaIn2S4molar content of 30% exhibits the optimum photocatalytic activity. The primary reason for the significantly enhanced photoreduction activity is proved to be the substantially improved separation efficiency of photogenerated electrons/holes caused by forming the CaIn2S4/ZnIn2S4heterostructured composites. The efficient charge separation can be evidenced by steady-state photoluminescence spectra (PLs) and transient photocurrent response. Based on the charge transfer between CaIn2S4and ZnIn2S4, an enhancement mechanism of photocatalytic activity and stability for the Cr(VI) reduction is proposed.Keywords:CaIn2S4/ZnIn2S4composites;Cr(VI);photocatalysis;simulated sunlight;hydrothermal method
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Chao Peng,Yiming Chen,Xingyue Gao,Ping Wei,Yihao Lin,Li Fu,Bingpu Zhou,Mengchen Zhang,Jianbo Jia,Tiangang Luan
In this study, leveraging the tunable surface groups of MXene , the two-dimensional (2D) Nb 2 C T x with OH terminal (NC) was synthesized. 2D ZnIn 2 S 4 (ZIS) nanosheets were prepared with the aid of sodium citrate, enhancing the exposure ratio of active (1 1 0) facet. On this basis, 2D/2D ZnIn 2 S 4 /Nb 2 C T x heterojunctions were fabricated to improve photocatalytic hydrogen evolution reaction (HER) performance. The optimized 6 wt%Nb 2 C T x /ZnIn 2 S 4 -450 (6NC/ZIS-450) photocatalyt exhibits a remarkable HER rate of 3603 μmol g −1 h −1 , which is 10 times superior to that of the original ZnIn 2 S 4 . Its apparent quantum efficiency (AQE) at 380 nm reaches 14.9 %. Meanwhile, even after 5 rounds of HER, the activity of 2D/2D ZnIn 2 S 4 /Nb 2 C T x heterojunction remained at 90 %, far superior to that of pure ZnIn 2 S 4 (34 % and 31 %). Energy band structure analysis and density functional theory (DFT) calculation indicate that Nb 2 C T x adsorbed with OH exhibit a low work function . By serving as a hole cocatalyst, it effectively boosts the photocatalytic HER rate of ZnIn 2 S 4 /Nb 2 C T x heterojunction and inhibits the photocorrosion of ZnIn 2 S 4 . This unique insight, via hole transport highways and increased exposure of active facets, effectively enhances the activity and stability of sulfides photocatalysts .
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TALANTA
·
2025
·
IF 6.1
Chunfang Wang,Rui Dai,Ziying Zhong,Faqiong Zhao,Baizhao Zeng
Developing effective detection methods for disease markers is essential for clinical diagnosis and therapeutic prognostic assessment. In this work, hollow Bi-doped Bi 2 WO 6 was synthesized by using carbon sphere as template, and then it was used as the label of secondary antibody to induce current polarity reversal in the flower shaped ZnIn 2 S 4 based photoelectrochemical (PEC) immunosensor. Thus the easily disturbed anodic photocurrent was converted to cathodic photocurrent with better resistance to interference from reducing substances. Furthermore, the reversal of polarity made the influence of background signal decrease, the detection range become wide, and the sensitivity increase. The introduced poly(dopamine) film could inhibit the anodic photocurrent of ZnIn 2 S 4 in addition to fixing antibody, assisting Bi 2 WO 6 in inducing subsequent current polarity conversion. Under the optimized conditions, the linear response range of the sandwich immunosensor was as wide as 0.0005−20.0 ng/mL, with a quite low limit of 0.18 pg/mL for the assay of model molecule carcinoembryonic antigen. The PEC sensor also exhibited satisfying selectivity and stability. It was applied to detect serum samples and satisfactory results were achieved.
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MICROCHEMICAL JOURNAL
·
2024
·
IF 4.9
Yiting Lei,Bingjie Pan,Gaiping Li,Lina Zou,Qi Shen
Residues of oxytetracycline (OTC) may cause the resistance of bacteria, and even have serious impacts on the ecosystem through the food chain. It was important to monitor OTC of low concentration for preserving human health and environmental safety. In this work, reduced graphene oxide doped ZnIn 2 S 4 (ZnIn 2 S 4 /rGO) nanocomposites were composited by straightforward one-step solvothermal reaction. The nanocomposites had superior light absorption property and stable photocurrent response. Because rGO not only had a large specific surface area for immobilizing abundant ZnIn 2 S 4 , but also accelerated charge transfer as an electron mediator. Additionally, the oxidation potential of OTC was more negative than the valence band potential of ZnIn 2 S 4 . So, OTC can be oxidized by photogenerated holes of the ZnIn 2 S 4 as electron donors, leading significant increase of photocurrent response. Based on this, a “signal-on” photoelectrochemical (PEC) sensor was constructed to achieve ultra-sensitive and specific detection of OTC. This sensor exhibited a wide detection range from 100 fM to 50 nM, an extremely low detection limit (61.2 fM) and excellent analytical performance in actual water, food and biological samples.
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GREEN CHEMISTRY
·
2024
·
IF 9.3
Qi Zhu,Bo Gong,Shuquan Huang,Yangxin Jin,Shengqin Liu,Shan Shao,Yuwei Yang,Taren Cataldo,Nicholas M. Bedford,Jason Chun-Ho Lam
The electrochemical selective oxidative transformation of lignin feedstocks into valuable oxygenated aromatics is essential to establish a sustainable biorefinery. In this study, we used a rhombohedral ZnIn2S4 (R-ZIS) electrocatalyst to realise the efficient anodic cleavage of C–O bonds in benzyl phenyl ether (BPE), an α-O-4 lignin model compound, to a series of industrially relevant oxygenated mono-aromatics. The reaction occurred at +2 VAg/AgCl, 65 °C, and atmospheric pressure. In optimised conditions, the reaction achieved over 99% conversion rate with a Faraday efficiency of 51.6% at 91.3% conversion of BPE, that is greater than most known electrocatalytic oxidative cleavage examples. The ZnIn2S4 electrocatalyst was deposited on a carbon cloth support, and its structural properties and surface morphology were extensively investigated. Systematic potential controlled electrolysis coupled with 18O isotopic labelling confirmed that C–O scission occurred exclusively between the benzylic carbon and phenolic oxygen. Furthermore, substrate competition studies were conducted to compare the electrocatalytic performance of the R-ZIS catalyst with that of its structural analogue, hexagonal ZnIn2S4, in terms of BPE and mono-aromatics conversion. The experimental results were supported by density functional theory calculations. The substrate scoping study revealed the suitability of the R-ZIS induced electrocatalytic system for a variety of substituted α-O-4/β-O-4 model dimers. Overall, this work demonstrates an efficient anodic process that can enable the atom-efficient valorisation of lignin to produce oxygenated aromatics. The proposed approach can complement the numerous existing reductive lignin cleavage methods.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
·
IF 9.7
Shuang Li,Shu-Zhao Sun,Zhi-Wen Wang,Ying-Zhang Shi,Yu-Jie Song,Ling Wu
Constructing dual single-atom catalysts with distinct electronic structures holds significance for the design of catalytic active centers, yet it remains highly challenging. Here, a novel light-induced approach was created to construct Ni 0 and Ni δ+ dual single-atom sites on ZnIn₂S₄ nanosheets (Ni 0 -Ni δ+ /ZIS) for the photocatalytic reduction of CO₂. Characterizations and density functional theory (DFT) calculations results indicate that Ni δ+ and Ni 0 single-atom sites can be selectively anchored in the Zn vacancies and lattice interstitials on the surface of ZIS, respectively. Ni 0 atoms are in a low-spin state without unpaired electrons. In contrast, Ni δ+ atoms are in an intermediate-spin state with an unpaired electron, which can be migrated from the 3d orbital of N δ+ to the 2π u orbitals of CO₂. Ni δ+ and Ni 0 sites decouple the competitive pathways of CO₂ reduction and H₂ evolution via distinct adsorption of H₂O and CO₂ on Ni 0 or Ni δ+ sites (ΔG > 0.5 eV), respectively. Ni 0 sites facilitate the generation of H₂ from H₂O, whereas Ni δ+ sites preferentially reduce CO₂ to CO. Furthermore, the Ni 0 -Ni δ+ dual single-atom sites significantly enhance the efficiency of charge separation and transfer. Therefore, the catalyst attains a high syngas yield of 58.66 mmol·g −1 ·h −1 under visible light, with adjustable CO/H₂ ratios from 1:1.3 to 1:4.1. This work presents a promising light-induced strategy for constructing dual single-atom catalysts via modulating metal electronic structure.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Tengfei Bao,Chenxi Tang,Shuming Li,Ping She,Heng Rao,Jun-sheng Qin
Dual Z-schemed photocatalysts possess superior charge-separation efficiency and powerful redox capabilities, which have attracted significant attention in photocatalytic CO 2 reduction (PCR). However, most of the dual Z-scheme systems are focused on inorganic semiconductors, which remain a challenge to control the selectivity of PCR products. Herein, we designed a cascade dual Z-scheme structured organic/inorganic heterojunction of HCdS@ZnIn 2 S 4 -Cobalt porphyrin (HCdS@ZIS-CoTPPS). HCdS@ZIS-CoTPPS demonstrated excellent PCR activity (CO rate: 93.64 μmol·g −1 ·h −1 ) and adjustable syngas ratio when compared to HCdS, ZIS, CoTPPS, and HCdS/ZIS. Experimental characterizations and density functional theory (DFT) calculations reveal that the superior PCR activity of HCdS@ZIS-CoTPPS is contributed by the broad light absorption range, short charge carrier migration path, low interface contact resistance, and strong redox ability induced by the hollow structured cascade dual Z-scheme heterojunction. This article provides valuable inspiration for the design and preparation of atomistic heterojunctions for solar-driven fuel generation.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Qingjie Luan,Xiangdong Xue,Hongtai Feng,Lu Tao,Dongxue Zhou,Tengfei Chen,Mengxi Tan,Wenjun Dong
Molecular-type cocatalysts can achieve the maximum electron transfer and minimum light absorption loss by virtue of their size advantage. Herein, a novel hydrophilic molecule-semiconductor hybrid P 4 @Vs-ZnIn 2 S 4−x photocatalyst was successfully developed by in-situ P 4 molecular anchoring on S defect ZnIn 2 S 4−x (V S -ZnIn 2 S 4−x ). The electron-rich P 4 molecules are anchored on the Zn-S 4 surface through S vacancies, forming Zn-P and S-P bonds that can promote electron injection from the electron-rich P 4 molecular to Vs-ZnIn 2 S 4−x substrate and reduce the adsorption/desorption barrier of H intermediate on S atom of Zn-S 4 plane. Meanwhile, the electrostatic potential depression around P 4 promoted the directional migration of in-plane photogenerated electrons, and pooled electrons to the highly active P sites and S sites, thereby accelerating the kinetics of hydrogen evolution. As a result, P 4 @Vs-ZnIn 2 S 4−x achieves an optimal photocatalytic hydrogen evolution activity of 26.1 mmol g −1 h −1 under visible light, which is 6.2 times higher than 4.2 mmol g −1 h −1 for Vs-ZnIn 2 S 4−x .
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