JOURNAL OF ALLOYS AND COMPOUNDS
·
2022
·
IF 6.371
Haoxiang Zhong,Lingzhi Zhang
The low sulfur utilization and the serious shuttle effect of polysulfides severely hamper practical application of Li-S batteries. Herein, sulfur cathodes with the multi-functional structures, featured with double-layered hollow carbon sphere with up to 50 nm interlayer space (DLHC-50) in situ grown Co-SnS catalytic layer is designed and synthesized for lithium sulfur batteries. Co-SnS/DLHC-50 can encapsulate 72% sulfur, higher than 63% for Co-SnS/DLHC-20 due to the large interlayer spaces of DLHC-50. Meanwhile, polysulfides are also effectively restricted via physical entrapment from DLHC-50 as well as chemical binding between Co-SnS and polysulfides. Benefiting from the well-constructed host framework, Co-SnS/DLHC-50 @S shows higher specific capacity/capacity retention of 760.4 mA h g −1 /72.9% after 500 cycles at 0.5 C, than that of 546.5 mA h g −1 /62.2% and 668.9 mA h g −1 /62.2%, for DLHC-50 @S, and Co-SnS/DLHC-20 @S, respectively. In addition, the strategy can be also extended to prepare other metal oxides (sulfides)/DLHC-50 for wide applications. Therefore, this work demonstrates a promising route to combat some bottlenecks such as low sulfur utilization, and the shuttle effect of polysulfides for Li-S batteries.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
·
IF 6.2
Xiaowei Chen,Zhongqin Li,Jiancheng Zhou,Shi Chen,Yi Huang,Weiwei Wang,Wuyou Wang,Qi Xu,Xinguo Xi
It is an effective strategy to improve photocatalytic degradation performance by constructing step scheme (S-scheme) heterojunction photocatalysts with superior photo-redox capacity and high charge transfer efficiency. In this study, a series of two-dimensional/two-dimensional (2D/2D) La 2 Ce 2 O 7 /g-C 3 N 4 (LCO/CN) S-scheme heterojunction photocatalysts were synthesized via in-situ solid-phase sintering by regulating the mass ratio of raw materials. The large junction area between La 2 Ce 2 O 7 nanosheets and ultra-thin graphitic carbon nitride (g-C 3 N 4 ) endows the composite with significantly enhanced separation and transfer efficiency of photogenerated carriers within a satisfactory light response region. The LCO/CN-2 composite not only shows the highest photocatalytic activity with a reaction rate constant of 0.02701 min −1 to degrade Rhodamine B (RhB) under visible light irradiation for 90 min but also demonstrates stable reusability after four runs. Moreover, based on the Mott-Schottky calculations, radical trapping experiments, and ESR analysis,·O 2- and·OH are identified as the main active species, and an S-scheme charge transfer mechanism is suggested to explain the enhanced photocatalytic activity. This work inspires the application of fluorite-type photocatalysts to wastewater purification and environmental restoration.
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CATALYSIS LETTERS
·
2023
·
IF 2.8
Liu Xinyu,Xu Jing,Li Faqin,Liu Zhenlu,Xu Shengming
With the increasing scarcity of resources, the search for green and available energy has become an urgent need. Among them, photocatalytic decomposition of water to hydrogen production has been widely studied. According to zeta potential and XRD characterization, NiCo2O4 and CuS were successfully reassembled by electrostatic self-assembly to construct S-scheme heterojunction induced by built-in electric site, which can accelerate the reaction. At the same time, under simulated visible light irradiation, the composite catalyst can rapidly decompose aqueous triethanolamine solution to produce hydrogen. The composite catalyst has high photocatalytic activity and shows a durable and efficient hydrogen generation effect. By studying the photogenerated carrier separation and transfer of the catalyst, the results show that the composite catalyst can accelerate the photogenerated carrier separation and transfer, so that it can participate in the photocatalytic reaction faster. It provides various insights into the construction of different heterojunctions in binary composite catalysts. Graphical Abstract
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Houfeng Zhang,Bojing Sun,Junjie Wang,Qian Zhu,Dongfang Hou,Chen Li,Xiu-qing Qiao,Dong-sheng Li
Optimize the separation and transport mechanism of photogenerated carriers in heterojunction composites, and make full use of the active sites of each material are key factors to enhance photocatalytic activity. Herein, we successfully synthesize defective CdLa 2 S 4 @La(OH) 3 @Co 3 S 4 (CLS@LOH@CS) Z-scheme heterojunction photocatalysts through a facile solvothermal method, which show broad-spectrum absorption and excellent photocatalytic activity. La(OH) 3 nanosheets not only greatly increase the specific surface area of photocatalyst, but also can be coupled with CdLa 2 S 4 (CLS) and form Z-scheme heterojunction by converting irradiation light. In addition, Co 3 S 4 with photothermal properties is obtained by in-situ sulfurization method, which can release heat to improve the mobility of photogenerated carriers, and also be used as a cocatalyst for hydrogen production. Most importantly, the formation of Co 3 S 4 leads to a large number of sulfur vacancy defects in CLS, and thus improving the separation efficiency of photogenerated electrons and holes, and increasing the catalytic active sites. Consequently, the maximum hydrogen production rate of CLS@LOH@CS heterojunctions can reach 26.4 mmol g -1 h −1 , which is 293 times than pristine CLS (0.09 mmol g -1 h −1 ). This work will provide a new horizon for synthesizing high efficiency heterojunction photocatalysts through switching the separation and transport modes of photogenerated carrier.
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Small
·
2023
·
IF 13.3
Wanqing Zhang,Jie Ying,Hongwei Liu
Transition metal-based catalysts possess high catalytic activity for oxygen evolution reaction (OER). However, the preparation of high-performance OER electrocatalysts using simple strategies with a low cost still faces a major challenge. Herein, this work presents an innovative, in situ-induced preparation of the Fe 2 O 3 , FeS, and NiS nanoparticles, supported on carbon blacks (CBs) (denoted as Fe 2 O 3 -Fe(Ni)S/C) as a high-efficiency oxygen evolution electrocatalyst by employing biomineralization. Biomineralization, a simple synthesis strategy, demonstrates a huge advantage in controlling the size of the Fe 2 O 3 and Fe(Ni)S nanoparticles, as well as achieving uniform nanoparticle distribution on carbon blacks. It is found that the electrocatalyst Fe 2 O 3 -Fe(Ni)S/C-200 shows a good OER electrocatalytic activity with a small loading capacity, and it has a small overpotential and Tafel slope in 1 m KOH solution with values of 264 mV and 42 mV dec −1 , respectively, at a current density of 10 mA cm −2 . Additionally, it presents good electrochemical stability for over 24 h. The remarkable and robust electrocatalytic performance of Fe 2 O 3 -Fe(Ni)S/C-200 is attributed to the synergistic effect of Fe 2 O 3 , FeS, and doped-Ni species as well as its distinct 3D spherical structure. This approach indicates the promising applications of biomineralization for the bio-preparation of functional materials and energy conversion.
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Advanced Science
·
2023
·Vol. 11
·期 5
·2305439
·
IF 15.1
Fucheng Zhang,Huanhuan Dong,Yi Li,Dengjiang Fu,Lu Yang,Yupeng Shang,Qiuyang Li,Yuwen Shao,Wu Gang,Tao Ding,Tao Chen,Wenkun Zhu
Photo-assisted uranium reduction from uranium mine wastewater is expected to overcome the competition between impurity ions and U(VI) in the traditional process. Here, B-TiO 2 @Co 2 P-X S-scheme heterojunction with metal-oxygen-hydrogen (M-O-H) is developed insitu modification for photo-assisted U(VI) (hexavalent uranium) reduction. Relying on the DFT calculation and Hard-Soft-Acid-Base (HSAB) theory, the introduction of metal-oxygen-hydrogen (M-O-H, hard base) metallic bonds in the B-TiO 2 @Co 2 P-X is found to enhance the hydrophilicity and the capture capability for uranyl ion (hard acid). Accordingly, B-TiO 2 @Co 2 P-500 hybrid nanosheets exhibit excellent U(VI) reduction ability (>98%) in the presence of competing ions. By self-consistent energy band calculations and in-situ KPFM spectral analysis, the formation of the internal electric field between B-TiO 2 and Co 2 P at the heterojunction is proven, offering a strong driving force and atomic transportation highway for accelerating the S-scheme charge carriers directed migration and promoting the photocatalytic reduction of uranium. This work provides a valuable route to explore the functionally modified photocatalyst with high-efficiency photoelectron separation for U(VI) reduction.
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ACS Sustainable Chemistry & Engineering
·
2023
·
IF 8.4
Ran Li,Deliang Zhang,Huamao Chen,Shaozhen Wang,Yunyun Ling,Caihong Fang
Developing high-performance and low-cost electrocatalysts for the oxygen evolution reaction (OER) and urea oxidation reaction (UOR) is essential for hydrogen production. Herein, we prepared Zn,S-incorporated Fe,Co layered double hydroxide (ZnCoFeS–LDH) nanosheets on nickel foam via a two-step hydrothermal reaction. The attractive two-dimensional (2D) nanosheet morphology with ultrathin thickness offers abundant active sites, promotes the adsorption and desorption of intermediates on the surface, and also facilitates mass transportation. The electronic structure of ZnCoFeS–LDH was modified, which thus improves their conductivity, offers high-valence iron ions (Fe3+), and therefore intrinsically enhances their electrocatalytic properties. In particular, the constructed crystalline/amorphous interfaces benefit electron transfer between different phases. As a proof of concept, we examined the electrocatalytic performances of ZnCoFeS–LDH nanostructures to both the OER and UOR. As a result, the ZnCoFeS–LDH nanosheets exhibit excellent catalytic OER activity, with low overpotentials of 202, 217, 238, and 261 mV to achieve current densities of 10, 20, 50, and 100 mA cm–2, respectively, which are remarkably enhanced in comparison with that of commercial RuO2. Furthermore, they also demonstrate outstanding durability after long-term (48 h) and cycling (5000 cycles) measurements. Moreover, the ZnCoFeS–LDH nanosheets also possess superior UOR activity. The potentials were measured to be as low as 1.313, 1.334, 1.366, and 1.398 V to reach current densities of 10, 20, 50, and 100 mA cm–2, respectively, with high long-term stability after 20 h.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Na Zhou,Rui Wang,Kun Liu
The development of low-Pt bifunctional electrocatalysts with excellent performance for oxygen reduction reaction (ORR) and hydrogen evolution reaction (HER) is critical for the advancement of the hydrogen economy. Here, we have integrated low-loading Pt and Co metals into N, S doped porous carbon nanosheets to obtain composite catalysts encapsulating PtCo alloy nanoparticles (PtCo2@Co 9 S 8 / N -CNS and PtCo2@ N -CNS). The acquired PtCo nanoparticles, with dimensions of about 2.5 nm, are uniformly distributed and firmly anchored in N, S doped carbon nanosheets with large specific surface areas and rich pore structure, forming multiple active centers and effectively preventing the aggregation of metal nanoparticles. The PtCo2@Co 9 S 8 / N -CNS and PtCo2@ N -CNS display high ORR catalytic mass activity of 1.65 A mg Pt -1 and 1.01 A mg Pt -1 in 0.1 M HClO 4 . The PtCo2@ N -CNS catalyst exhibits excellent HER performance in 0.5 M H 2 SO 4 , with a mass activity (at 50 mV) 4.3 times higher than that of Pt/C. The PtCo2@Co 9 S 8 / N -CNS and PtCo2@ N -CNS also exhibit stronger ORR and HER stability than Pt/C after accelerated durability tests. The superior catalytic activity performance of catalysts can be attributed to the synergistic effect of multiple active centers of PtCo, Co 9 S 8 and Co-N in the catalysts. The confinement of PtCo nanoparticles by Co metal and N, S doped porous nanosheets derived from graphitic carbon nitride (g-C 3 N 4 ) as the template, which can effectively prevent the corrosion and migration of the catalysts under acidic conditions, enhances the catalytic stability of the materials. This study provides a new perspective for the development of economical and efficient bifunctional low-Pt catalysts.
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Shuai Zhang,Linxiang Yang,Gaoyu Liu,Shengli Zhang,Qingsong Shan,Haibo Zeng
I–III–VI quantum dots (QDs) and derivatives (I, III, and VI are Ag+/Cu+, Ga3+/In3+, and S2–/Se2–, respectively) are the ideal candidates to replace II–VI (e.g., CdSe) and perovskite QDs due to their nontoxicity, pure color, high photoluminescence quantum yield (PLQY), and full visible coverage. However, the chaotic cation alignment in multielement systems can easily lead to the formation of multiple surface vacancies, highlighted as VI and VVI, leading to nonradiative recombination and nonequilibrium carrier distribution, which severely limit the performance improvement of materials and devices. Here, based on Zn–Ag–In–Ga–S QDs, we construct an ultrathin indium sulfide shell that can passivate electron vacancies and convert donor/acceptor level concentrations. The optimized In-rich 2-layer indium sulfide structure not only enhances the radiative recombination rate by preventing further VS formation but also achieves the typical DAP emission enhancement, achieving a significant increase in PLQY to 86.2% at 628 nm. Moreover, the optimized structure can mitigate the lattice distortion and make the carrier distribution in the interior of the QDs more balanced. On this basis, red QD light-emitting diodes (QLEDs) with the highest external quantum efficiency (EQE; 5.32%) to date were obtained, providing a novel scheme for improving I–III–VI QD-based QLED efficiency.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Xuemei Li,Yang Shen,Fangyu Jin,Jingbo Zhang,Yanyan Yang,Xiaoshu Qu
Nuclear waste management and nuclear energy generation require the proper disposal of 129 I and 131 I, which are radioactive isotopes of iodine. For recognition of different types’ iodine, a magnetic poly (ionic liquid)s (Fe 3 O 4 @SiO 2 -MPS-PILs) was formed by the selected imidazole ionic liquid monomer and core–shell Fe 3 O 4 @SiO 2 -MPS via free radical polymerization. The resulting adsorbent containing plenty of imidazole N-heterocycle units, benzene rings, and ionic bonds in the backbones was suitable for simultaneously adsorbing iodine molecules and iodide ions. The adsorption mechanisms for iodine in cyclohexane and iodide ions from aqueous solution were based on charge transfer and ion exchange mechanisms, respectively. The adsorption equilibrium for iodine in cyclohexane was attained at 12 h, and the kinetics of iodine adsorption closely followed the pseudo-second-order model. Iodine adsorption on Fe 3 O 4 @SiO 2 -MPS-PILs was best described by Langmuir model with a maximum iodine adsorption capacity of approximately 714.29 mg g −1 . Iodide ions adsorption was best explained with Freundlich model and a maximum adsorption capacity of 335.80 mg g −1 was achieved in an iodide solution with a 500 mg L –1 concentration. Notably, Fe 3 O 4 @SiO 2 -MPS-PILs retained over 90 % of its original adsorption performance after the 5th cycle. This work proves that the adsorbent Fe 3 O 4 @SiO 2 -MPS-PILs was efficient and recyclable, and has good application prospects in the practical treatment of iodine and iodide.
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Nanoscale
·
2021
·Vol. 13
·期 24
·10849-10861
·
IF 7.79
Shunyou Hu,Yuanyuan Hu,Xiangli Liu,Jiaheng Zhang
Lithium–sulfur (Li–S) batteries generally suffer from a serious “shuttle effect” during the charging/discharging process, resulting in the loss of active components and sluggish redox reaction kinetics that hinder the cycle life and rate performance of the battery. To address this, CoSe/C hollow structures (CoSe/C HSs) were prepared via a simple hydrothermal strategy and used as a sulfur host for Li–S batteries. The battery with CoSe/C HSs exhibited a high initial specific discharge capacity of 1405 mA h g−1 with a coulombic efficiency of 99.8% at 0.1C. Additionally, S@CoSe/C HS cathodes with a high sulfur loading of 5.1 mg cm−2 delivered a considerable specific discharge capacity of 1256.1 mA h g−1 and maintained a high capacity of 1120 mA h g−1 after 100 cycles with a capacity decay rate of 0.11% per cycle at 0.1C. The unique raspberry-like structure of CoSe/C HSs prevents polysulfides from escaping the cathode host via both physical containment and the formation of Co–S and Se–Li chemical bonds, and it also enhances the polysulfide redox kinetics. Furthermore, the peculiar raspberry-like structure can withstand volume changes during charging/discharging to better protect the cathode.
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Acta Pharmaceutica Sinica B
·
2021
·
IF 11.614
Boyi Niu,Yixian Zhou,Kaixin Liao,Ting Wen,Sixian Lao,Guilan Quan,Xin Pan,Chuanbin Wu
The therapeutic efficacy of cisplatin has been restricted by drug resistance of cancers. Intracellular glutathione (GSH) detoxification of cisplatin under the catalysis of glutathione S -transferases (GST) plays important roles in the development of cisplatin resistance. Herein, a strategy of “pincer movement” based on simultaneous GSH depletion and GST inhibition is proposed to enhance cisplatin-based chemotherapy. Specifically, a redox-responsive nanomedicine based on disulfide-bridged degradable organosilica hybrid nanoparticles is developed and loaded with cisplatin and ethacrynic acid (EA), a GST inhibitor. Responding to high level of intracellular GSH, the hybrid nanoparticles can be gradually degraded due to the break of disulfide bonds, which further promotes drug release. Meanwhile, the disulfide-mediated GSH depletion and EA-induced GST inhibition cooperatively prevent cellular detoxification of cisplatin and reverse drug resistance. Moreover, the nanomedicine is integrated into microneedles for intralesional drug delivery against cisplatin-resistant melanoma. The in vivo results show that the nanomedicine-loaded microneedles can achieve significant GSH depletion, GST inhibition, and consequent tumor growth suppression. Overall, this research provides a promising strategy for the construction of new-type nanomedicines to overcome cisplatin resistance, which extends the biomedical application of organosilica hybrid nanomaterials and enables more efficient chemotherapy against drug-resistant cancers.
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