CHEMICAL RESEARCH IN CHINESE UNIVERSITIES
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2021
·Vol. 38
·期 1
·200-208
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IF 1.307
Wang Yue,Wang Xiaoxue,She Ping,Guan Dehui,Song Lina,Xu Jijing
D esign and fabrication of functional porous air cathode materials with superior catalytic activity is still the key point for non-aqueous lithium-oxygen(Li-O 2 ) batteries. Herein, inspired by the self-standing three-dimensional(3D) structure of the natural spinach leaves, a unique binder-free and self-standing porous Au/spinach cathode for high-performance Li-O 2 batteries has been developed. The carbonized spinach leaves serve as a superconductive current collector and an ideal porous host for accommodating catalysts. The Au/spinach cathode could offer enough spaces for accommodating the discharge products, shorten the distance of the oxygen and electrolyte diffusion, and promote the oxygen reduction reaction(ORR) and oxygen evolution reaction (OER) processes. This optimized Au/spinach cathode achieved a high specific area capacity of 7.23 mA·h/cm 2 at a current density of 0.05 mA/cm 2 and exhibited excellent stability(280 cycles at 0.05 mA/cm 2 with a fixed capacity of 0.2 mA·h/cm 2 ). The superior performance encourages the construction of more advanced cathode architectures by the use of bio-composites for Li-O 2 batteries.
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ACS Sustainable Chemistry & Engineering
·
2020
·
IF 7.632
Zhengyi Qian,Xudong Li,Liguang Wang,Tianpin Wu,Baoyu Sun,Lei Du,Yulin Ma,Chunyu Du,Pengjian Zuo,Geping Yin
Rechargeable aprotic Li–O2 batteries have drawn much attention in light of their ultrahigh theoretical energy density. However, the sluggish kinetics of oxygen cathode reactions lead to huge energy loss, while the unfavorable side reactions associated with the widely used carbon and binder account for fast battery decay during cycles. Herein, hierarchically holey IrNi alloy nanosheets are facilely designed on Ni foam substrate as a freestanding, binder- and carbon-free cathode to address these challenges. The IrNi nanosheets consist of numerous interconnected nanoparticles, forming abundant nanoholes, benefiting active-site exposure. Moreover, the meso-/macropores pave channels for the transfer of oxygen and lithium ions and provide enough accommodation for the insoluble Li2O2 product. The corresponding Li–O2 batteries demonstrate low polarization and excellent cycle stability with full discharge/charge capability (up to 292 cycles at a current density of 0.2 mA cm–2 within a voltage range from 2.3 to 4.3 V). The long-term cycling performance is principally attributed to the exclusive catalytic stability of the holey IrNi nanosheets and its good compatibility with dimethyl sulfoxide-based electrolyte. Our research provides novel insights into the design of robust and freestanding porous cathodes for high energy density Li–O2 batteries.
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ACS Applied Energy Materials
·
2020
·
IF 4.473
Jia Liu,Ying Wang,Dan Zhou,Dan Li,Ziye Kang,Haiming Xie
Although a redox mediator (RM) strategy can lower the overpotential of Li–O2 batteries (LOBs), the redox shuttling results in an undesired RM consumption and a continued decomposition of lithium metal anode, leading to a poor cycling stability. In this work, a hybrid inorganic–organic composite separator based on polyethylene oxide/TiO2/polypropylene (PEO/TiO2/PE) in LOBs has been reported for the first time, which aims to suppress the RM shuttling. The influences of TiO2 nanoparticles and PEO on battery performance are systematically investigated. Benefiting from the synergistic advantages, a LOB with PEO/TiO2/PE separator displays stable cyclability, considerable rate performance, and good reversibility. Additionally, the mechanism of inhibiting shuttling effect by this composite separator is proposed. We hope that this work can give an insight into the development of multiple functional separators for Li anode protection in LOBs.
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Journal of Materials Chemistry A
·
2020
·Vol. 8
·期 19
·9813-9824
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IF 11.301
Yue Li,Jian Song,Mengting Jiang,Mbage Bawa,Xiaohong Wang,Yuyang Tian,Guangshan Zhu
Na5[IMo6O24]·3H2O and a porous aromatic framework (iPAF-1) were used to build an off-the-shelf building material (IMo6@iPAF-1) to realize the highly efficient oxidation of organic sulfurs like oxygenase. The synergy between IMo6 and iPAF-1 resulted in a higher BET surface area, hydrophobic microenvironment, and redox sites to show higher activity in aerobic oxidative desulfurization with almost 100% removal of model organic sulfurs under atmospheric pressure with almost 246 times higher TOFs compared to IMo6. It also showed efficiency in the desulfurization of gasoline and diesel to give very low S contents of 7.1 and 7.6 ppm with 99.3% and 99.4% removal, respectively, at 100 °C for 6 h. More importantly, IMo6@iPAF-1 could also catalyze desulfurization using concentrated O2 mixed with N2 or air instead of pure O2 with better safety and economics, while as low as 4.9 and 6.9 ppm S contents were achieved for gasoline and diesel, respectively. The special surroundings of IMo6@iPAF-1 repelled the sulfone product and allowed it to perform with the same efficiency when recycled without any treatment of the used catalyst.
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JOURNAL OF HAZARDOUS MATERIALS
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2020
·
IF 9.038
Yong Liu,Ni Tan,Jinrui Guo,Jianlong Wang
In this study, a novel Al°-CNTs-Cu 2 O composite, capable of activating O 2 to generate H 2 O 2 and further to reactive oxygen species (ROSs) at a wide pH range, was synthetized, characterized and applied for the degradation of sulfamerazine. In the activation of O 2 by Al°-CNTs-Cu 2 O composite, H 2 O 2 was generated from the reaction of O 2 with Al°-CNTs, which could be catalytically decomposed into O 2 − and OH by Cu 2 O, the formed Cu(II) could be rapidly reduced to Cu 2 O by Al°-CNTs in composite, which made Al°-CNTs-Cu 2 O composite reusable and decreased the leaching of copper ions into solution. The removal efficiency of SMR and TOC was 73.91 % and 56.80 %, respectively at initial pH = 5.8, T = 20 °C, O 2 flow rate = 100 mL/min, Al°-CNTs-Cu 2 O dosage = 2 g/L, SMR = 50 mg/L, and reaction time = 60 min. The removal efficiency of SMR kept almost unchanged and the concentration of copper ions in solution was below 0.5 mg/L. The Al°-CNTs-Cu 2 O/O 2 process could be used as a novel catalyst for the degradation of refractory organic contaminants in water and wastewater by Fenton-like process at a wide pH range through the in situ generation of H 2 O 2 .
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PubMed
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2020
·Vol. 44
·期 27
·11808-11816
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IF 3.288
Shi-Yuan Zhang,Jing-Jing Ma,Hong-Lin Zhu,Yue-Qing Zheng
Syngas, as a necessary feedstock dependent on non-renewable fossil fuels, is a mixture of CO and H2, which could be prepared by a renewable strategy via electrochemical CO2 reduction in water electrolyte solutions. Herein, beaded Au@Co3O4 nanowire arrays (denoted as Au@Co3O4 NAs) were obtained by immersion in HAuCl4 solution with Co3O4 nanowire arrays. The Au@Co3O4 NAs exhibited outstanding electrochemical performance of producing syngas via tuning from 1 : 1 to 4 : 1 with controlling voltage. In addition, the Au@Co3O4 NAs showed better catalytic performance for the oxygen evolution reaction with an overpotential of 320 mV at a current density of 50 mA cm−2, along with a small Tafel slope of 75 mV dec−1 in 1 M KOH solution. The electrochemical performance of Au@Co3O4 NAs is obviously superior to Co3O4 NAs, which will open up a viable strategy for the design and fabrication of a bi-functional electrocatalyst for the overall reaction (CO2 + H2O → CO + H2 + O2).
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Yu Luo,Chenchen Liu,Jiahui Liu,Xueming Liu,Yang Zhou,Xinwen Ou,Bo Weng,Jin Jiang,Bin Han
Photocatalytic O 2 reduction presents a sustainable strategy for H 2 O 2 synthesis, while the in-situ decomposition of H 2 O 2 significantly deteriorates the activity and stability. Here, by introducing anthraquinone centers into covalent organic frameworks (DQTb-COFs), for the first time, we realized the suppression of in-site decomposition of generated H 2 O 2 via site-engineering of COFs. Under visible light irradiation, DQTb-COFs achieves an H 2 O 2 generation rate of 1844.1 μmol h −1 g −1 without sacrificial agents, which is about 3.4 times that of its counterpart without anthraquinone centers (DATb-COFs). The generated H 2 O 2 on DATb-COFs is readily reduced into hydroxyl radicals (•OH), which is not observable on DQTb-COFs. Experiments and calculations demonstrated that the anthraquinone centers of DQTb-COFs can enhance the generation of H 2 O 2 by facilitating the utilization of O 2 and promoting the desorption of H 2 O 2 . This work highlights how to inhibit the in-situ decomposition of H 2 O 2 via site-engineering of COFs, and blazes a new trail for highly efficient H 2 O 2 photosynthesis.
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Journal of Materials Chemistry A
·
2015
·Vol. 4
·期 4
·1399-1407
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IF 7.443
Guangyu Zhao,Li Zhang,Jixian Lv,Changle Li,Kening Sun
Hydrothermal self-assembly is a highly efficient and low cost method to prepare graphitic foam from graphene oxides; however, the self-assembly frameworks usually do not have controllable pore structures because of the spontaneous process. In this paper, a hydrothermal synthesis assisted by ammonium peroxo-polymolybdate [(NH4)2Mo2O11] tailoring to fabricate graphitic foam is presented. The foam possesses pore structures which can be controlled by adjusting the rate of charge in the hydrothermal experiments. Furthermore, the foam obtained from a definite rate of charge [(NH4)2Mo2O11 : graphene oxide is 1 : 2 in weight] has a hierarchical pore structure and a through-hole net. In electrochemical energy storage, such unique features are beneficial for providing efficient mass transport as well as abundant, accessible active sites. The graphitic foam was tested for use as self-supported electrodes of Li–O2 batteries (LOBs) and Li ion batteries (LIBs) without any metallic current collectors or organic binders, and the foam frameworks exhibited remarkable lithium ion storage properties in both of the two batteries (e.g., 5500 mA h g−1 at 0.2 A g−1 as LOB cathodes and 250 mA h g−1 at 50 A g−1 as LIB anodes).
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ACS Applied Nano Materials
·
2024
·
IF 5.3
Xiang Yu,Yuwei Mi,Zihan Gong,Yongfang Zhang,Lei Wang,Suyuan Zeng
Constructing heterojunctions is an effective strategy for increasing semiconductor photocatalytic activity. Herein, a Bi2O3/Bi4O5Br2 type-II heterojunction was synthesized using a simple one-pot solvothermal route. The 0-dimensional (0D) Bi2O3 nanoparticles are uniformly distributed within the 2D Bi4O5Br2 nanosheets with (101̅) facets dominantly exposed. In comparison with pure Bi2O3 and Bi4O5Br2, they show higher photocatalytic activity degradation of resorcinol (RO) and Rhodamine B (RhB). The Bi2O3/Bi4O5Br2 composite containing 10% Bi2O3 (BOB4) displays the best photocatalytic activity. For instance, compared with pure Bi4O5Br2 and Bi2O3, the k(RO) values of BOB4 (0.58 h–1) are 3.1 and 4.8 times higher. The enhanced photocatalytic activity is attributed to the formation of a large heterojunction interface that results from the homogeneous distribution of Bi2O3 nanoparticles in the Bi4O5Br2 nanosheet, which effectively enhances the photogenerated charge separation in a type-II mode. Major active species include superoxide radicals (•O2–), hydroxyl radicals (•OH), and holes (h+). In addition, the Bi2O3/Bi4O5Br2 photocatalysts exhibit outstanding resistance to inorganic ions, pH, water matrix, as well as outdoor sunlight and favorable stability and biocompatibility. This work presents a simple method to construct Bi-based heterojunction architectures for photoactivity improvement.
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CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Wei Du,Zhihua Zhang,Jundi Wang,Nan Song,Xuezhi Duan,Xinggui Zhou
Propylene epoxidation by H 2 and O 2 to propylene oxide (HOPO), as a novel method for PO production, has attracted widespread attention due to its economic and environmental advantages. Acrolein is a notable byproduct arising in HOPO reaction over Au/TS-1 catalyst, and is traditionally thought to be exclusively formed on Au site through propylene oxidation. However, on the intraporous and external surface Au sites of Au-Ti catalysts, the HOPO reaction have been shown to proceed by different mechanisms, yet the effect of active sites distribution on acrolein formation is far from being understood. Herein, we found that the reaction orders in acrolein formation on Au/TS-1 catalyst (H 2 , 0.19; O 2 , 0.44; C 3 H 6 , 0.44) relative to Au/TS-1 with blocked pores (Au/TS-1-B) catalyst (H 2 , −0.36; O 2 , 0.61; C 3 H 6 , 0.52) were quite different, suggesting a variation in the reaction pathway on the catalysts with different Au locations. Moreover, it is found that PO can be converted to acrolein by O 2 on TS-1 zeolite, which is absent on TS-1-B zeolite without micropores. Consequently, acrolein formation on Au/TS-1 catalyst can proceed through two parallel pathways: propylene hydro-oxidation on Au site, and PO conversion by O 2 inside micropores. Furthermore, by designing and preparing the Au/TS-1 catalysts with different structures, the Au locations are closely related to acrolein formation mechanism and kinetic behaviors. This work provides kinetic insights into the acrolein formation pathways in the HOPO reaction on Au/TS-1 catalyst, and is helpful to the rational design and preparation of efficient catalysts with high selectivity.
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Chemical Science
·
2024
·
IF 7.6
Yinglei Tao,Tao Wang,Xingyu Yu,Ke Gong,Hao Gong,Haixia Chen,Xiaoli Fan,Aidi Zhang,Xianli Huang,Kun Chang,Jianping He
Li–O2 batteries (LOBs) boast an exceptionally high theoretical energy density; however, the slow kinetics of the oxygen electrode reaction have been a significant hurdle in their advancement and practical application. In this study, a composite of bismuth oxyhalide heterojunction incorporated with metal–organic frameworks (MOFs) was engineered on carbon cloth (Zr-MOF/BiOIBr/CC) as an efficient bifunctional catalyst to enhance the oxygen electrode reaction in photo-assisted LOBs. Compared to Zr-MOF/CC, Zr-MOF/BiOIBr/CC significantly expands the light absorption spectrum of the catalyst. Furthermore, the built-in electric field in the heterojunction aids in the separation and directional movement of photogenerated carriers, thereby expediting the reaction kinetics of LOBs. Consequently, the photo-assisted LOBs with Zr-MOF/BiOIBr/CC as the cathodes display a discharge potential of 3.05 V, a low charge potential of 3.20 V, and an energy efficiency of up to 95.3%, and can sustain an extended cycle life of over 255 cycles. This study underscores the potential application of MOFs/semiconductor heterostructural materials in photo-assisted LOBs and offers insights into the systematic design of photo-assisted air batteries and other advanced semiconductors.
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Energy & Environmental Materials
·
2025
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IF 14.1
Zhengcai Zhang,Dulin Huang,Xiaohui Peng,Zhang Zhang,Yaying Dou,Zhen Zhou
Redox mediators (RMs) represent the most promising strategy to address the sluggish kinetics of lithium–oxygen (Li–O 2 ) batteries. To achieve high-energy and cost-effective Li–O 2 batteries, carbon materials are typically regarded as ideal cathodes in these systems. However, the impact of their surface properties—which often regulate specific discharge pathways—on the RM-mediated oxygen reduction reaction (ORR) remains unclear. In this study, CNTs electrodes with different surface properties are fabricated. Results suggest that CNTs with more surface defects not only promote the unmediated discharge pathway even in RMs-involved battery systems but also exacerbate the corrosion of carbon cathodes. This, in turn, leads to the undesired accumulation of Li 2 O 2 and Li 2 CO 3 on the cathode surface, which hinders effective and continuous electron transfer between the cathode and RMs, ultimately decreasing the catalytic activity of RMs. As a result, the discharge capacity of the battery is seriously diminished, especially at large current densities. These findings underscore the significance of surface engineering in advancing the performance of RMs-assisted Li–O 2 batteries.
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