Small
·
2023
·Vol. 19
·期 33
·2301391
·
IF 13.3
Wenjing Zhang,Jian Zheng,Ruoyu Wang,Li Huang,Junkai Wang,Tianran Zhang,Xiangfeng Liu
Lithium–oxygen (Li–O 2 ) batteries have received extensive attention owing to ultrahigh theoretical energy density. Compared to typical discharge product Li 2 O 2 , LiOH has attracted much attention for its better chemical and electrochemical stability. Large-scale applications of Li–O 2 batteries with LiOH chemistry are hampered by the serious internal shuttling of the water additives with the desired 4e − electrochemical reactions. Here, a metal organic framework-derived “water-trapping” single-atom-Co-N 4 /graphene catalyst (Co-SA-rGO) is provided that successfully mitigates the water shuttling and enables the direct 4e − catalytic reaction of LiOH in the aprotic Li–O 2 battery. The Co-N 4 center is more active toward proton-coupled electron transfer, benefiting - direction 4e − formation of LiOH. 3D interlinked networks also provide large surface area and mesoporous structures to trap ≈12 wt% H 2 O molecules and offer rapid tunnels for O 2 diffusion and Li + transportation. With these unique features, the Co-SA-rGO based Li–O 2 battery delivers a high discharge platform of 2.83 V and a large discharge capacity of 12 760.8 mAh g −1 . Also, the battery can withstand corrosion in the air and maintain a stable discharge platform for 220 cycles. This work points out the direction of enhanced electron/proton transfer for the single-atom catalyst design in Li–O 2 batteries.
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高影响因子
ACS Applied Materials & Interfaces
·
2019
·
IF 8.456
Junfang Ding,Liping Li,Haorui Zheng,Ying Zuo,Xiyang Wang,Huixia Li,Shaoqing Chen,Dan Zhang,Xingliang Xu,Guangshe Li
Nanomaterials are widely used as redox-type reaction catalysts, while reactant adsorption and O2 activation are hardly to be promoted simultaneously, restricting their applications in many important catalytic fields such as preferential CO oxidation (CO-PROX) in H2-rich stream. In this work, an interface-enhanced Co3O4–CuCoO2 nanomesh was initially synthesized by a hydrothermal process using aluminum powder as a sacrificial agent. This nanomesh is systematically characterized by powder X-ray diffraction, scanning electron microscopy, transmission electron microscopy, N2 adsorption, X-ray photoelectron spectroscopy, UV–vis absorption spectroscopy, Raman spectroscopy, X-ray absorption near-edge spectroscopy, hydrogen temperature-programmed reduction, and oxygen temperature-programmed desorption. It is demonstrated that the nanomesh possesses high-density nanopores, enabling a large number of CO adsorption sites exposed to the surface. Meanwhile, electron transfer from O2– to Co3+/Co2+ and the weakened bonding strength of Co–O bond at surfaces promoted the oxygen activation and redox ability of Co3O4. When tested as a catalyst for CO-PROX, this nanomesh with an optimized pore structure and a surface electronic structure, exhibits a strikingly high catalytic oxidation activity at low temperatures as well as a broader operation temperature window (i.e., CO conversion >99.0%, 100–200 °C) in the CO selective oxidation reaction. The present finding should be highly useful in promoting the quest for better CO-PROX catalysts, a hot topic for proton exchange membrane fuel cells and automotive vehicles.
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高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2018
·Vol. 26
·期 2
·1445-1454
·
IF 2.8
Wang Daiyao,Zou Jing,Cai Huahua,Huang Yixin,Li Fei,Cheng Qingfeng
Advanced oxidation processes offer effective solutions in treating wastewater from various industries. The process of alkali-activated hydrogen peroxide (H 2 O 2 ) was superior for the treatment of alkaline dye wastewater because no additional reagents were required except H 2 O 2 . However, an important and interesting phenomenon had been observed that the primary reactive species were found different for degrading organic pollutants with the process of alkali-activated H 2 O 2 . Azo dye of Orange G (OG) and triphenylmethane dye of Rhodamine B (RhB) were chosen as the target organic pollutants. The influences of various parameters on OG and RhB degradation by alkali-activated H 2 O 2 were evaluated. Furthermore, different scavengers, including ascorbic acid, methanol, t -butanol, isopropyl alcohol, furfuryl alcohol, and nitro blue tetrazolium, have been tested to identify the active species involved in dye degradation, and it was found that O 2 ·− was mainly responsible for degrading OG, while HO 2 − anion was the primary oxidant for degrading RhB.
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高影响因子
ACS Applied Energy Materials
·
2018
·
IF 0
Huanhuan Guo,Guangmei Hou,Jianguang Guo,Xiaohua Ren,Xiaoxin Ma,Linna Dai,Shirui Guo,Jun Lou,Jinkui Feng,Lin Zhang,Pengchao Si,Lijie Ci
Lithium–oxygen batteries (LOBs) have attracted increasing interest because of their superior theoretical specific energy. However, the stability of lithium metal anode is one of the obstacles limiting their practical applications. Here, we introduce an artificial Li3PO4 solid electrolyte interphase (SEI) film to protect the lithium anode in LOB with LiI/LiNO3/DMSO (dimethyl sulfoxide) electrolyte. The Li3PO4-protected Li anode exhibits excellent electrochemical stability during the Li stripping/plating process and leads to a relatively uniform and featureless surface in LOB after cycling. Our research demonstrates that superior electrochemical performance can be achieved in the Li–O2 battery with the synergistic combination of the DMSO-based electrolyte, the LiI redox mediator, and the Li3PO4-protected Li anode. The LOB with a Li3PO4-protected Li anode exhibits a prolonged cycling life span of 152 cycles with a fixed capacity of 1000 mA h g–1 at 2 A g–1. The results in this work provide knowledge for the development of a robust strategy for protecting the Li anode in the applications of Li–O2 batteries.
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RSC Advances
·
2018
·Vol. 8
·期 41
·23397-23403
·
IF 2.936
Zhuo-Liang Jiang,Jing Xie,Cong-Shan Luo,Meng-Yang Gao,Huan-Liang Guo,Mo-Han Wei,Hong-Jun Zhou,Hui Sun
The mechanism of Li–O2 batteries is based on the reactions of lithium ions and oxygen, which hold a theoretical higher energy density of approximately 3500 W h kg−1. In order to improve the practical specific capacity and cycling performance of Li–O2 batteries, a catalytically active mechanically robust air cathode is required. In this work, we synthesized a freestanding catalytic cathode with RuO2 decorated 3D web Co3O4 nanowires on nickel foam. When the specific capacity was limited at 500 mA h g−1, the RuO2–Co3O4/NiF had a stable cycling life of up to 122 times. The outstanding performance can be primarily attributed to the robust freestanding Co3O4 nanowires with RuO2 loading. The unique 3D web nanowire structure provides a large surface for Li2O2 growth and RuO2 nanoparticle loading, and the RuO2 nanoparticles help to promote the round trip deposition and decomposition of Li2O2, therefore enhancing the cycling behavior. This result indicates the superiority of RuO2–Co3O4/NiF as a freestanding highly efficient catalytic cathode for Li–O2 batteries.
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高影响因子
AICHE JOURNAL
·
2022
·Vol. 69
·期 5
·e17999
·
IF 4.167
Dong Lin,Yang Xu,Xiuhui Zheng,Wei Sheng,Zhenyi Liu,Yinglong Yan,Yu Cao,Yibin Liu,Xiang Feng,De Chen,Chaohe Yang
Regulating the microenvironment of active sites is crucial to boost the performance of direct propene epoxidation with H 2 and O 2 . Herein, the enhanced surface transfer of H 2 O 2 intermediates was first achieved by sodium-decorated Au-Ti bifunctional active sites. Combined with multi-techniques (e.g., operando UV–vis–NIR system, DFT studies and quantitative model calculations), it is found that the sodium-decorated silanols (Si-ONa species) on the TS-1 support enhance the formation of Ti-OOH intermediates by restraining H 2 O 2 decomposition. In addition, sodium-decorated silanols improves the desorption of propylene oxide, suppressing its ring-opening and formation for the carbonaceous deposits. Moreover, the sodium-decorated Au nanoparticles with smaller diameter and higher electron density further strengthen O 2 adsorption and boost the H 2 O 2 formation. This work not only provides fundamental understandings on the microenvironment of Au-Ti bifunctional catalysts but also sheds new light on enhancing the performance by boosting the surface molecular transfer.
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高影响因子
Energy Technology
·
2022
·Vol. 10
·期 12
·2200800
·
IF 4.149
Haoxiang Zhong,Qianqian Hu,Lingzhi Zhang
The shuttle effect of polysulfides severely limits the practical application of lithium–sulfur batteries. Herein, the lithium-rich Li[Li 0.2 Ni 0.2 Mn 0.6 ]O 2 /hierarchical porous graphitic carbon composite (LLNM/HPGC) is designed and synthesized as host material for lithium–sulfur batteries, aiming to restrict the shuttle effect of polysulfides via physical entrapment from 3D HPGC and accelerate the conversion of polysulfides from the lithium-rich LLNM as catalyst. Benefiting from the well-constructed host framework, 1glycerinum-LLNM/2HPGC@sulfur (1Gly-LLNM/2HPGC@S) shows higher specific capacity of 651 mAh g −1 after 200 cycles at 0.5C than that of 546.3, 422.8, 476, and 421.7 mAh g −1 for HPCG@S, Gly-LLNM@S, 1Gly-LLNM/3HPGC@S, and 1Gly-LLNM/5HPGC@S. Therefore, this work demonstrates a promising route to inhibit the shuttle effect of polysulfides for lithium–sulfur batteries.
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高影响因子
Catalysis Science & Technology
·
2021
·Vol. 11
·期 23
·7632-7639
·
IF 6.119
Hongjiao Wang,Bo Fan,Zhongkuan Luo,Qixing Wu,Xuelong Zhou,Fang Wang
The development of high-performance cathodes is critical to promoting the development of Li–O2 batteries. In this work, three-dimensional NiCo2O4 nanowire-decorated NiO nanosheets (NiO@NiCo2O4) on a Ni foam were fabricated by a two-step solvothermal process. The product exhibited efficient catalytic performance for Li–O2 batteries. This three-dimensional NiO@NiCo2O4 hierarchical structures grown on Ni foam forms a porous catalytic surface for the uniform growth of discharge products. First, NiCo2O4 is a promising catalyst for improving the oxygen reduction reaction/oxygen evolution reaction (ORR/OER) processes for the Li–O2 batteries. Second, NiO can provide a porous scaffold for the further deposition of NiCo2O4 nanowires to avoid their aggregation. Furthermore, NiO can promote the decomposition of by-products containing carbonate/carboxylate species. As a result, the Li–O2 system with NiO@NiCo2O4 as a carbon-free cathode showed a maximum in-depth-specific discharge capacity of 9361.4 mA h g−1 at a current density of 100 mA g−1 and 176 cycles of stability under a limited capacity of 500 mA h g−1 at a current density of 200 mA g−1. The reported strategy regarding a multicomponent hierarchical structure may provide a new approach for effective electrocatalyst design for Li–O2 batteries.
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高影响因子
ACS Sustainable Chemistry & Engineering
·
2021
·
IF 8.198
Lei Shi,Gan Wang,Jian Li,Meifen Wu,Zhaoyin Wen
The practical applications of Li–O2 batteries are hindered by the large charge polarization. Recently, the development of redox mediators (RMs) brings new hope for constructing low overpotential Li–O2 batteries. However, the “shuttle effect” of RMs causes new problems. Here, based on a low-cost and environmentally friendly biomaterial–bacterial cellulose, a sulfonation strategy was adopted to produce a functional gel polymer electrolyte for LiI-involved Li–O2 batteries. Benefiting from the high-density negatively charged sulfonate groups on the sulfonated bacterial cellulose, the functionalized gel electrolyte can produce strong electrostatic repulsion force to the negatively charged I3– ions to suppress the shuttle effect. As a result, the Li–O2 battery shows a good cycling performance with eliminated self-discharge, and the Li anode is successfully protected by the inhibition of I3– shuttling. This novel approach may provide new insights into the development of functionalized gel polymer electrolytes for Li–O2 batteries with redox mediators.
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高影响因子
BIOMATERIALS
·
2021
·
IF 12.479
Hua Yu,Yue Cheng,Cong Wen,Yi-Qing Sun,Xue-Bo Yin
Nanozymes have been combined with glucose oxidase (GOx) for dual-enzyme cascade catalytic therapy. However, their catalysis efficiency is restricted because of the hypoxia tumor microenvironment (TME). Although many methods are developed for O 2 supply, the O 2 leakage and consumption of H 2 O 2 compromised their practical application. Herein, a biocompatible carbon nitride (C 3 N 4 )/nanozyme/GOx triple cascade nanocatalyst was designed with laser-activatable O 2 self-supply via water splitting to relieve tumor hypoxia and thus improve the catalysis efficiency. To this end, polydopamine (PDA) nanosphere was prepared and attached with C 3 N 4 nanosheet to improve water splitting efficiency and realize photothermal-enhanced catalysis, simultaneously. The [email protected] 3 N 4 composite was then coated with MIL-100 (Fe), where GOx was loaded, to form C 3 N 4 /MIL-100/GOx triple cascade nanocatalyst. The triple cascade catalysis was realized with laser-activatable O 2 supply from [email protected] 3 N 4 , H 2 O 2 generation with GOx, and •OH production from peroxidase-like MIL-100 (Fe) for tumor therapy. Upon 808 nm irradiation, PDA, as a photothermal agent, realized photothermal therapy and enhanced the catalytic therapy. Thus, the synergy of laser-activatable O 2 supply and photothermal enhancement in our triple cascade nanocatalyst improved the performance of catalytic therapy without drug resistance and toxicity to normal tissues.
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高影响因子
Biomaterials Science
·
2021
·Vol. 9
·期 20
·6772-6786
·
IF 6.843
Sulan Luo,Yiting Zhao,Kewei Pan,Yixian Zhou,Guilan Quan,Xinguo Wen,Xin Pan,Chuanbin Wu
The low oxygen level in tumors significantly reduces the antitumor efficacy of photodynamic therapy (PDT). The provision of O2 and monomeric hydrophobic photosensitizers (PSs) under physiological conditions would greatly help to shrink malignant tumors. We take advantage of the high porosity and multifunctionality of metal–organic frameworks (MOFs) to fabricate a simple all-in-one nanoplatform mediated by microneedle delivery to achieve synergistic O2 evolution and chemophototherapy. An iron(III)-based MOF (MIL-100(Fe)) acted not only as a vehicle for the concurrent delivery of zinc phthalocyanine (ZnPc) and doxorubicin hydrochloride (Dox), but also to supply O2 by decomposing hydrogen peroxide (H2O2) in the tumor microenvironment via a Fenton-like reaction. In vitro and in vivo experiments indicated that the nanoplatform had excellent biocompatibility and exerted enhanced anticancer effects. The encapsulated drug was sustainably released from the nanoplatform skeleton in response to acidic tumor microenvironments. Moreover, upon 660 nm light irradiation, ZnPc effectively produced reactive oxygen species (ROS) due to the reduction of hypoxia by MIL-100(Fe). A microneedle technique was adopted to directly deliver the nanoplatform into superficial tumors rather than via systemic circulation. Hence, this study provides a new strategy for more efficient chemophototherapy of hypoxic superficial tumors.
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高影响因子
JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
·
2021
·Vol. 32
·期 2
·2026-2040
·
IF 2.478
Zhang He,Qian Jianhua,Zhang Jie,Xu Jiasheng
TiO 2 @Sn(Sb)O 2 core–shell composites (TiO 2 @SnO 2 , TiO 2 @Sb 2 O 4 and TiO 2 @Sb-SnO 2 ) have been prepared through a chemical co-precipitation method with a calcination process. The mixture hydrolysates of SnCl 4 and SbCl 3 have been deposited on the surface of TiO 2 as the precursor. These hydrolysates have been converted to Sn(Sb)O 2 particles, leading to the formation of the TiO 2 @Sn(Sb)O 2 core–shell structure. Their electrochemical performances and electrocatalytic degradation efficiencies of methylene blue (MB) have been investigated. It is found that TiO 2 @Sb-SnO 2 electrode presents a larger effective electrocatalytic area and more electroactive sites, which provide more contact points between the pollutant and electrode and enhance electrocatalytic oxidation activity. The TiO 2 @Sb-SnO 2 electrode exhibits a higher degradation efficiency (97.6%) than that of TiO 2 @SnO 2 (80.1%) and TiO 2 @Sb 2 O 4 (34.9%). The TiO 2 @Sb-SnO 2 electrode provides a 91.1% degradation efficiency after five cycles test, indicating a high stability during degradation process. These results show that the as-prepared TiO 2 @Sb-SnO 2 electrode can provide a promising application to treat dye wastewater, which relies on its core–shell structure.
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高影响因子
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