CATALYSIS TODAY
·
2025
·
IF 5.3
Jun Wu,Qi Li,Keke Zhang,Shuailing Wang,Xianjun Lang,Feng Wang
Linear conjugated polymers have emerged as a versatile class of visible light photocatalysts, attracting increasing interest due to their tunable optoelectronic properties. However, their linear backbones often result in insufficient electron transfer, a limitation that can be mitigated by coupling them with a conductive π-conjugated system such as reduced graphene oxide (rGO). Here, we report the electrostatic self-assembly of a dibenzothiophene- S , S -dioxide-based conjugated polymer (PSOBN2) with rGO, forming a PSOBN2-rGO heterostructure. The two-dimensional conjugated structure of rGO facilitates π-electron transfers over PSOBN2 through interfacial coupling, thereby overcoming the inherent charge carrier transport limitation of linear conjugated polymers for enhanced charge separation and accelerated interfacial electron transfer. An optimized heterostructure, PSOBN2-rGO1, exhibits a better H 2 O 2 production rate of 9972 μmol h –1 g –1 in an air atmosphere under visible light irradiation, which is 1.42 times that of pristine PSOBN2. Notably, under natural sunlight irradiation, PSOBN2-rGO1 demonstrates an exceptional H 2 O 2 production rate of 9267 μmol h –1 g –1 within the initial hour. Mechanistic studies confirm the crucial role of rGO-facilitated electron transfer in promoting the reduction of O 2 and oxidation of H 2 O dual pathways for the photosynthesis of H 2 O 2 . This work offers a strategy for overcoming the inherent limitations of linear conjugated polymers toward efficient artificial photosynthesis of H 2 O 2 .
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ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Lixiong Xu,Shuo Geng
Electrocatalytic glycerol oxidation reaction (GOR) coupled with hydrogen evolution reaction (HER) is an ideal method to achieve efficient hydrogen production. However, realizing the stable degradation of glycerol to formate at high current densities still faces great challenges, mainly stemming from the competition between GOR and oxygen evolution reaction (OER) at high potentials. To address this issue, in this study, S–Cu–Ni/NF catalysts were successfully synthesized using Cu–Ni/NF catalysts as precursors. The introduction of Cu effectively suppressed the OER, enabling the catalysts to achieve more than 75% formate Faraday efficiency over a wide potential range from 1.3 V vs RHE to 1.6 V vs RHE. Meanwhile, S doping significantly enhanced the electron transport ability of GOR, enabling the S–Cu–Ni/NF catalyst to achieve a high current density of 100 mA cm–2 at a low potential of 1.395 V vs RHE. In addition, after 24 h of continuous operation at a high current density of 100 mA cm–2, the catalyst potential increased by only 40 mV, demonstrating excellent stability. Scanning electron microscopy with energy dispersive spectra (SEM-EDS), X-ray photoelectron spectra (XPS) and in situ Raman characterization confirmed that the precipitation of S promoted the formation of the active site NiOOH and its dynamic growth during the GOR process. The present study not only improved the selectivity of formate at high potentials by inhibiting OER but also significantly enhanced the GOR performance, demonstrated the potential of stable degradation of glycerol at high current densities, and provided a feasible strategy for the industrial application of glycerol oxidation coupled with hydrogenolysis.
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LETTERS IN APPLIED MICROBIOLOGY
·
2021
·Vol. 72
·期 4
·399-407
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IF 2.858
Wang N.,Xu Y.,Peng C.,Wang X.,Wei Y.,Li K.,Wang S.,Xu A.,Gao J.
A strain NQ1, which showed efficient asymmetric reduction of 3,5‐bis(trifluoromethyl) acetophenone (BTAP) to enantiopure (S)‐[3,5‐bis(trifluoromethyl)phenyl]ethanol ((S)‐BTPE), which is the key intermediate for the synthesis of a receptor antagonist and antidepressant, was isolated from a soil sample. Based on its morphological and internal transcribed spacer sequence, the strain NQ1 was identified to be Rhodotorula mucilaginosa NQ1. Some key reaction parameters involved in the bioreduction catalyzed by whole cells of R. mucilaginosa NQ1 were subsequently optimized, and the optimized conditions for the synthesis of (S)‐BTPE were determined to be as follows: 5·0 ml phosphate buffer (200 mmol l−1, pH 7·0), 80 mmol l−1 of BTAP, 250 g (wet weight) l−1 of resting cell, 35 g l−1 of glucose and a reaction for 18 h at 30°C and 180 rev min−1. The strain NQ1 exhibited a best yield of 99% and an excellent enantiomeric excess of 99% for the preparation of (S)‐BTPE under the above optimal conditions, and could also asymmetrically reduce a variety of bulky prochiral carbonyl compounds to their corresponding optical hydroxyl compound with excellent enantioselectivity. These results indicated that R. mucilaginosa NQ1 had a good capacity to reduce BTAP to its corresponding (S)‐BTPE, and might be a new potential biocatalyst for the production of valuable chiral hydroxyl compounds in industry.
研究领域:
微生物学
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生物催化
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有机化学
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2022
·
IF 5.518
Yan Wang,Shengzhe Zhao,Yi Yang,Raul D. Rodriguez,Anya Lipovka,Yun Lu,Honglan Huang,Jinju Chen
Ag nanoparticle-decorated Bi 2 O 3 -TiO 2 heterogeneous photocatalysts were successfully obtained by combining facile sacrificial templates and photoreduction . The as-synthesized Ag@Bi 2 O 3 -TiO 2 photocatalysts with a narrow band gap of 2.40 eV exhibited considerable photocatalytic activity to degrade rhodamine B (RhB) and tetracycline hydrochloride (TCH), and the removal efficiency reached 100% and 92%, respectively. Ag@Bi 2 O 3 -TiO 2 photocatalysts also exhibited stable recyclability for the degradation of RhB and TCH. Trapping experiments helped determine the major reactive oxidative species for TCH photodegradation . The desirable photodegradation performance is mainly attributed to improved light absorption , enhanced charge separation, and strong redox capacity of Ag@Bi 2 O 3 -TiO 2 nanostructures with S-scheme heterojunction . This work provides a facile avenue to construct heterogeneous tubular nanostructures with intensive photoabsorbance and effective photocatalysis to degrade organic contaminants.
研究领域:
材料科学
·
环境科学
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Lijuan Chen,Yaoyong Dong,Mengwei Han,Ting Song,Xuejun Zheng,Wenyuan He,Bei Long,Xiongwei Wu,Yong Pei,Xianyou Wang
MnOOH is regarded as a product of manganese-based materials after H + insertion. There is rare study on the Zn 2+ /H + storage capability of MnOOH. Herein, MnOOH nanofibers are prepared through a one-step hydrothermal method and developed as a promising cathode. The introduction of S doping changes the crystal structure of MnOOH and is conducive to its electronic/ionic transport and structural stability, proven by density functional theory calculations and various characterizations. The reduced Zn 2+ diffusion barrier of S-doped MnOOH leads to its increased Zn 2+ storage capability in the test of rate capability, especially at large current density. The Zn 2+ /H + insertion-type mechanism of MnOOH is revealed by ex situ XRD, Raman, XPS, and SEM tests. Therefore, this optimized material delivers a high reversible capacity of 178 mAh g −1 at 0.1 A g −1 , a good rate capability of 50 mAh g −1 at 3.0 A g −1 , and a long cyclic life with 108 mAh g −1 at 0.5 A g −1 over 500 cycles. Moreover, the electrode still shows satisfactory rate capability and cyclic life even at the high mass loadings of 10 and 15 mg cm −2 . This work proves the Zn 2+ /H + storage capability of MnOOH and its potential as a high-performance cathode in aqueous zinc ion battery.
研究领域:
材料科学
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电化学
·
能源存储
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INORGANIC CHEMISTRY
·
2022
·
IF 5.436
Zhijie Zhang,Liang Li,Ying Jiang,Jiayue Xu
Heterojunction manipulation has been deemed as a promising approach in exploring efficient photocatalysts for CO2 reduction. In this article, a novel step-scheme (S-scheme) photocatalyst of CsPbBr3 quantum dots/BiOBr nanosheets (CPB/BiOBr) was fabricated via a facile self-assembly process. The strong interaction, staggered energy band alignments, and much different Fermi levels between CsPbBr3 and BiOBr promised the formation of an S-scheme heterojunction. The resultant CPB/BiOBr heterojunction delivered remarkable photocatalytic performance in CO2 reduction, with an electron consumption rate of 72.3 μmol g–1 h–1, which was 4.1 and 5.7 times that of single CsPbBr3 and BiOBr, respectively. The superior photocatalytic performance originated from the impactful spatial separation of photoinduced electron–hole pairs, as well as the preservation of strongly reductive electrons for CO2 reduction. This work offers a rational strategy to design S-scheme heterojunctions based on lead halide perovskites, which are expected to have potential applications in the field of photocatalysis and solar energy utilization.
研究领域:
材料科学
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环境科学
·
化学工程
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SOLAR ENERGY
·
2021
·
IF 5.742
Ting Wang,Jiayong Zhang,Bin Yao,Yongfeng Li,Zhanhui Ding,Chunkai Wang,Jia Liu
Five types of Cu 2 ZnSn(S,Se) 4 (CZTSSe) films were fabricated by selenization of Cu 2 ZnSnS 4 (CZTS) precursor films preparing through Cu-Zn-Sn-S precursor solutions with nominal Cu + /(Cu + +Cu 2+ ) ratio of 0, 0.2, 0.4, 0.8 and 1. Five types of CZTSSe solar cells were prepared by using the five types of CZTSSe films as absorbers, respectively. The crystal quality and phase composition of the CZTS and CZTSSe films were characterized by XRD, Raman and SEM, and the photovoltaic performance for the CZTSSe solar cells were measured by J-V and EQE. It is found that the CZTS film consists of kesterite CZTS when the ratio is 0 and of kesterite CZTS together with a small amount of SnS when the ratio is 0.2 to 1. All of the CZTSSe films are comprised of kesterite CZTSSe and a small amount of Zn(S,Se). The crystal quality and lattice constants of the kesterite CZTSSe increase with increasing the ratio, while the amount of Zn(S,Se) decreases with increasing the ratio and almost to zero as the ratio is 1. The power conversion efficiency ( PCE ) of the CZTSSe solar cells increases from 5.47% to 8.43% as the ratio increases from 0 to 1, which is due to improvement in short-circuit current density ( J sc ) and filling factor ( FF ) and decrease in open circuit voltage deficit ( V oc , def ). The influence mechanism of the ratio on the PCE is suggested by analyzing effect of the ratio on electrical parameters of the CZTSSe solar cells.
研究领域:
光伏技术
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材料科学
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半导体薄膜
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太阳能电池技术
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ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Yubo Hu,Yuxiang Liu,Jun Wu,Yuda Li,Jiaxing Jiang,Feng Wang
Most of the traditional polymeric photocatalysts are generally insoluble in organic solvents, which might exclude their compatibility with large-area processing technology. Herein, we have synthesized a novel quaternized ammonium conjugated polyelectrolyte (PSO-FNBr) that can be processed to prepare an active film by a drop-casting method. PSO-FNBr shows a remarkably enhanced hydrogen evolution rate (HER) of 20.5 mmol h–1 g–1 in the thin film form in comparison to that of the powder form. Furthermore, we prepared a new type of thin film-based photocatalytic device, which provided a rare example of a “three-in-one” (rapid sampling + easy-to-use + cost-effective) photocatalytic system. The PSO-FNBr thin film over the Pt substrate can maintain a competitive HER, even though the Pt substrate was recycled and reused 50 times. Considering the features of impressive activity and low cost, we believe that PSO-FNBr will be a promising material for potential application in photocatalysis.
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ACS Applied Materials & Interfaces
·
2020
·
IF 8.758
Xing Yu,Weiwei Zhang,Lu Liu,Yves Fautrelle,Xionggang Lu,Xi Li
The abundant mass and charge transfer involved in Faradaic redox reactions are largely determined by microstructures including the surface area and porosity, elemental composition and electrical conductivity of bimetallic sulfides. Here, a high magnetic field (HMF) was introduced to tune these intrinsic characters for superior supercapacitor electrodes. We developed a novel HMF-controlled anion-exchange methodology to prepare the one-dimensional (1D) bunched Zn–Co–S yolk–shell balls (ZCS6T BYSBs). The HMF-induced directional growth and alignment of Zn0.76Co0.24S drive the directional 1D assembly. The as-obtained ZCS6T BYSBs possess larger surface area/pore volume, higher crystallinity and electrical conductivity, richer electroactive elements, and favorable axial electron and ion transport because of HMF-enhanced favorable ion diffusion and exchange kinetics. Flexible S, N codoped carbon nanotubes/graphene films embedded with the ZCS6T BYSBs (CZS6T/CNTs/SNGS) were fabricated by vacuum filtration and one-step S, N codoping and reduction of graphene oxides to improve structural stability and charge transport. The CZS6T/CNTs/SNGS electrode displayed impressive enhanced specific capacitance and rate capability with 78.7% capacitance retention at 30 A g–1. Furthermore, the CZS6T/CNTs/SNGS//CNTs/SNGS asymmetric supercapacitor delivered remarkable cycling stability with a high energy density of 41.1 W h kg–1 at a large power density of 9022 W kg–1.
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ACS Sustainable Chemistry & Engineering
·
2020
·
IF 7.632
Lu Chen,Li−Li Cui,Zizhun Wang,Xingquan He,Wei Zhang,Tewodros Asefa
Efficient, durable, nonprecious metal-based catalysts for electrochemical reactions involving oxygen are needed to advance the widespread use of fuel cells and Zn-air batteries. In this work, hybrid materials composed of bimetallic (Co and Fe) sulfide (Co8FeS8) nanoparticles supported on N,S-doped carbon microparticles that can serve as dual-function oxygen electrocatalysts are synthesized. The synthesis of the materials is performed by preparing and then pyrolyzing silica-protected Fe- and Co-modified, S-containing polyphthalocyanine at different temperatures. The materials are named (Fe,Co)SPPc-T-sp, where T denotes the pyrolysis temperature and sp represents the silica protection applied for their synthesis. Among them, the material synthesized at 900 °C, denoted (Fe,Co)SPPc-900-sp, shows superb electrocatalytic activities in an alkaline solution both toward the oxygen reduction reaction (ORR), with a half-wave potential (E1/2) of 0.830 V vs RHE, and toward the oxygen evolution reaction (OER), with a current density of 10 mA cm–2 at an overpotential (η10) of 353 mV. The catalytic activities of this material for both reactions are comparable with those of the respective benchmark, precious-metal-based catalysts, namely, Pt/C (20 wt %) and RuO2, respectively. An alkaline Zn-air battery assembled using (Fe,Co)SPPc-900-sp as an air electrode delivers a high peak power density (158.6 mW cm–2) and outstanding charge–discharge cycling stability (for over 50 h). These catalytic performances are better than those of the corresponding battery containing Pt/C and RuO2 electrocatalysts. This work also offers a facile synthetic strategy for the fabrication of robust, inexpensive dual-function electrocatalysts for Zn-air batteries.
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JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY B-BIOLOGY
·
2016
·
IF 3.035
Hang Yang,Guangying Hou,Li Zhang,Lei Ju,Chunguang Liu
Sewage sludge , as a very significant sources of BPS (up to 523 mg/kg dw) introduction into the environment, must be handled properly. Therefore, it is important to access BPS removal and its effect on sludge treatment with the biological treatment. However, it is unclear for its effect on the hydrolysis of sludge. In this research, impact of BPS on sludge hydrolysis by α-Amylase is studied from the respect of component of soluble organic matter in sludge using three-dimensional fluorescence spectra . Enzyme activity assay suggests that sludge hydrolysis is inhibited due to the denaturation of α-Amylase with BPS exposure. In order to illuminate the interaction mechanism between BPS and α-Amylase, UV–vis, steady-state fluorescence, circular dichroism , synchronous fluorescence, light scattering spectra, enzyme activity assay and molecule docking techniques are applied. Results show that BPS interacts with α-Amylase by hydrophobic bond in the activity region of α-Amylase. This interaction not only causes an unfolding skeleton structure of α-Amylase and a less hydrophobic microenvironment of tyrosine and tryptophan residues, but also leads to a specific fluorophore quenching involving static and dynamic type. This work provides direct evidence about enzyme toxicity of BPS and establishes a new strategy to investigate the interaction between protein and BPS at a molecular level, which is helpful for clarifying the bioactivities of BPS.
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Carbon Energy
·
2024
·
IF 19.5
Shengnan He,Hui Wu,Shuang Li,Ke Liu,Yaxiong Yang,Hongge Pan,Xuebin Yu
SnO 2 has been extensively investigated as an anode material for sodium-ion batteries (SIBs) and potassium-ion batteries (PIBs) due to its high Na/K storage capacity, high abundance, and low toxicity. However, the sluggish reaction kinetics, low electronic conductivity, and large volume changes during charge and discharge hinder the practical applications of SnO 2 -based electrodes for SIBs and PIBs. Engineering rational structures with fast charge/ion transfer and robust stability is important to overcoming these challenges. Herein, S-doped SnO 2 (S–SnO 2 ) quantum dots (QDs) (≈3 nm) encapsulated in an N, S codoped carbon fiber networks (S–SnO 2 –CFN) are rationally fabricated using a sequential freeze-drying, calcination, and S-doping strategy. Experimental analysis and density functional theory calculations reveal that the integration of S–SnO 2 QDs with N, S codoped carbon fiber network remarkably decreases the adsorption energies of Na/K atoms in the interlayer of SnO 2 –CFN, and the S doping can increase the conductivity of SnO 2 , thereby enhancing the ion transfer kinetics. The synergistic interaction between S–SnO 2 QDs and N, S codoped carbon fiber network results in a composite with fast Na + /K + storage and extraordinary long-term cyclability. Specifically, the S–SnO 2 –CFN delivers high rate capacities of 141.0 mAh g −1 at 20 A g −1 in SIBs and 102.8 mAh g −1 at 10 A g −1 in PIBs. Impressively, it delivers ultra-stable sodium storage up to 10,000 cycles at 5 A g −1 and potassium storage up to 5000 cycles at 2 A g −1 . This study provides insights into constructing metal oxide-based carbon fiber network structures for high-performance electrochemical energy storage and conversion devices.
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