JOURNAL OF POWER SOURCES
·
2024
·
IF 8.1
Wenyi Wang,Long Tang,Cheng Chen,Xueqin Wang,Yuanyuan Wang,Wencong Sun
Efficient and stable electrocatalysts with low platinum content are crucial for the practical application of fuel cells. The development of Pt-based single atom catalysts (SACs) has emerged as a promising research direction. In this study, we design and prepare a SACs based on MoS 2 with Pt–S–Mo and Pd–S–Mo active sites (Pd, Pt–MoS 2 ) by successively occupying vacancies, while maintaining the individual characteristics of the active sites. The resulting Pd, Pt–MoS 2 catalyst exhibits excellent electrocatalytic activity for oxygen reduction reaction (ORR), long-term stability, and resistance to common poisons (SCN − , S 2− , and methanol) under neutral conditions. Meanwhile, the microbial fuel cell (MFC) equipped with Pd, Pt–MoS 2 exhibits excellent performance in terms of actual electricity generation performance and sewage purification capacity with an ultrahigh power density, average chemical oxygen demand (COD) removal rate, and coulombic efficiency (CE) of 1398.6 ± 43.5 mW m −2 , 96.2 ± 2.2 %, and 22.5 ± 0.5 %, respectively. This strategy will provide new insights into the development of advanced bimetallic as well as polymetallic doped vacancies of MoS 2 SACs.
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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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PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2022
·Vol. 24
·期 12
·7521-7530
·
IF 3.945
Qixiao Gai,Shoutian Ren,Xiaochun Zheng,Wenjun Liu,Quanli Dong
Low-cost and high-abundance Cu nanostructures are potential near-infrared (NIR) surface plasmonic resonance (SPR) photosensitizers for carbon nitride (C3N4) photocatalysts, but their low activity and stability need to be improved. In this article, doping S into C3N4 (S-C3N4) creates anchoring sites for photo-deposited Cu nanoparticles (NPs), and the spontaneous construction of S-Cu bonds is realized between S-C3N4 and Cu NPs. The optimal hydrogen evolution rate of 1.64 mmol g−1 h−1 is obtained for S-C3N4–Cu, which is 5.5, 4.6 and 1.7 times that of pure C3N4, S-C3N4 and S-C3N4–Cu, respectively. With further loading of a Pt co-catalyst to confirm the role of Cu NPs and improve the photocatalytic activity of the SCN–Cu, the photocatalytic rate can reach up to 14.34 mmol g−1 h−1. Due to the NIR SPR effect of Cu NPs, the apparent quantum efficiency (AQE) of S-C3N4–Cu at 600 and 765 nm is 2.02% and 0.47%, respectively. The enhanced photocatalytic performance of S-C3N4–Cu compared with C3N4–Cu is mainly due to the introduced S–Cu bonds that improve the injection rate of hot electrons. This solution provides a simple and efficient interface optimization strategy for the construction of efficient NIR-driven photocatalysts.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2019
·
IF 14.229
Ge Shu,Yuda Li,Zhuang Wang,Jia-Xing Jiang,Feng Wang
Conjugated polymers have recently emerged as encouraging metal-free photocatalysts for solar energy conversion under visible light irradiation. Unfortunately, photocatalytic activities of the current polymers are still inadequate. Herein, we present a simple but quite attractive conjugated homopolymer (PDBTSO) based a dibenzothiophene-S,S-dioxide moiety. The introduction of sulphonyl group to a polyfluorene-like backbone can cause richly available active sites and lead to the efficient separation of photoexcited charge carriers, thus yielding impressive photocatalytic performance. Furthermore, we explored a natural “phosphorylation” strategy for increasing photocatalytic hydrogen production over PDBTSO. Remarkably, an extremely high hydrogen evolution rate of 44.2 mmol h −1 g −1 was achieved with the optimum addition of K 2 HPO 4 under visible light irradiation.
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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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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 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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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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JOURNAL OF POWER SOURCES
·
2024
·
IF 8.1
Kanglin Yu,Yuanyuan Xiao,Shiqi Hu,Xufan Zheng,Bowen Gao,Jingjing Xu,Zongzhe Li,Ruike Zhou,Yaowen Hu,Qingliang You,Biao Xiao,Renqiang Yang
Quantum dot (QD) based luminescent solar concentrator-organic photovoltaic (LSC-OPV) systems demonstrate significant potential in applications including building-integrated photovoltaics (BIPV). In this study, eco-friendly Ag–In–S/Zn–S QDs with a high photoluminescence quantum yield (PLQY = 73 %) are synthesized using a simple hydrothermal method. The influence of Zn-S precursor reactivity on QD properties is studied. The synthesized QDs exhibit excellent stability over a wide temperature range (90–360 K). The Ag–In–S/Zn–S LSCs maintain over 90 % of their initial PLQY after a two-month exposure to natural sunlight. Additionally, the power conversion efficiency (PCE) of the fabricated LSC-OPV system reaches 1.00 % under near-actual condition (9 mW cm −2 ). Moreover, when the irradiation intensity is further decreased to 0.4 mW cm −2 , the LSC-OPV system shows a PCE as high as 5.27 %, demonstrating that the LSC-OPV system can operate efficiently at low illumination intensities. Notably, the fabricated LSCs have minimal impact on the incident sunlight spectrum, making them suitable for BIPV applications. Thus, this study is a first that is known to report the integration of eco-friendly QD-based LSCs with organic photovoltaic cells, which positively contributes to the advancement of BIPV.
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ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Dongxu Zhang,Weixuan Dong,Yanhong Liu,Xiaoqing Gu,Tianyu Yang,Qiang Hong,Di Li,Dongqi Zhang,Hongbo Zhou,Hui Huang,Baodong Mao,Zhenhui Kang,Weidong Shi
Photoassisted electrocatalysis (P-EC) emerges as a rising star for hydrogen production by embedding photoactive species in electrocatalysts, for which the interfacial structure design and charge transfer kinetics of the multifunctional catalysts remain a great challenge. Herein, Zn-AgIn5S8 quantum dots (ZAIS QDs) were embedded into 2D NiFe layered double hydroxide nanosheets through a simple hydrothermal treatment to form 0D/2D composite catalysts for P-EC. With evidence from transient photovoltage spectroscopy, we acquired a clear and fundamental understanding on the kinetics of charge extraction time and extraction amount in the 0D/2D heterojunctions that was proved to play a key role in P-EC. Upon light illumination, for HER, the optimized NiFe-ZAIS exhibits obviously reduced overpotentials of 129 and 242 mV at current densities of 10 and 50 mA cm–2, which are 22 and 33 mV lower than those of dark electrocatalysis, respectively. For OER, the NiFe-ZAIS electrode also shows low overpotentials of 220 and 268 mV at current densities of 10 and 50 mA cm–2, respectively, under light illumination, which were able to almost double the intrinsic activity. Finally, with NF@NiFe-ZAIS as both the cathode and the anode, the assembled electrolyzer only requires 1.62 V to reach the overall water splitting current density of 10 mA cm–2 under P-EC. This work provides a useful example for the profound understanding of the design and the kinetics study of multifunctional P-EC catalysts.
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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.
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