Journal of Physical Chemistry C
·
2014
·
IF 4.835
Sujie Chang,Shigang Ruan,Erlong Wu,Weixin Huang
Oxide-on-metal particles with exposed interfaces exhibit wealthy structures and functions, but their facile synthesis remains as a challenge. Herein we report a facile O2-assisted hydrothermal method to synthesize CeO2-on-Ag particles with different CeO2 thicknesses. In this novel approach Ag particles catalyze the O2 + H2O reaction to form surface hydroxyls that induce the preferential nucleation of Ce(OH)3 on the surfaces of Ag particles, eventually forming CeO2 adlayers on Ag particles. CeO2-on-Ag particles exhibit the CeO2 thickness-dependent SERS effect in which their best SERS effect is 2 orders stronger than that of Ag particles. They also exhibit CeO2 thickness-dependent catalytic performance in CO oxidation in which the best one is as active as traditional CeO2-supported Ag catalyst. These results open up new opportunities to synthesize oxide-on-metal particles and explore their functions by tuning the oxide adlayer thickness.
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
GREEN CHEMISTRY
·
2014
·Vol. 17
·期 1
·335-342
·
IF 6.852
Muge Niu,Yucui Hou,Shuhang Ren,Wenhua Wang,Qitian Zheng,Weize Wu
Conversion of cellulose, the most abundant biomass, shows a high selectivity to yield formic acid (FA), when oxidized by O2 in NaVO3–H2SO4 aqueous solution. This conversion involves various reactions including hydrolysis and oxidation. In this work, the relationships between these reactions were studied. There are mainly two hydrolyses and two oxidations occurring in the conversion: initial hydrolysis (from cellulose to monosaccharides) and deep hydrolysis (from monosaccharides to levulinic acid); catalytic oxidation (from monosaccharides to FA) and ordinary oxidation (from levulinic acid to acetic acid). Among these four reactions, catalytic oxidation to FA and deep hydrolysis to byproducts are competitive. The increasing rate of deep hydrolysis is faster than that of catalytic oxidation, when temperature is increased. Catalytic oxidation is promoted and deep hydrolysis is suppressed, when the O2 pressure is increased. Moreover, deep hydrolysis is promoted and catalytic oxidation is suppressed, when H2SO4 concentration is increased. The hydrolysis–oxidation pathway of this conversion was proposed. Thus, the byproducts could be inhibited, and FA-oriented transformation could be realized.
研究领域:
生物化学
·
可再生能源
✓ 已验证
产品关联
DOI
高影响因子
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.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
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.
研究领域:
材料科学
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电化学
·
能源存储技术
✓ 已验证
产品关联
DOI
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.
研究领域:
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
PubMed
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.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
产品关联
DOI
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.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
BIOMATERIALS
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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.
研究领域:
纳米技术
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癌症治疗
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材料科学
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生物医学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Energy Storage Materials
·
2020
·
IF 16.28
Xiaohong Zou,Kaiming Liao,Di Wang,Qian Lu,Chuan Zhou,Ping He,Ran Ran,Wei Zhou,Wanqin Jin,Zongping Shao
Although aprotic Li-air batteries offer an attractive option for achieving ultrahigh energy density of electrochemical energy storage devices, the now-established system has so far fallen short of its potential due to a daunting challenge related to its open configuration, which results in not only the rapid corrosion of Li metal anodes but also the gradual evaporation of organic liquid electrolytes. Here, we show that these issues can be well addressed by protecting the Li-air battery with a new O 2 -permeable silica-aerogel-reinforced polydimethylsiloxane external membrane (OPSP). The highly flexible OPSP basically benefiting from hydrogen-bond cross-linking can be constructed in situ on any substrate with particularly desirable properties such as being water-/electrolyte-proof, O 2 -permeable, high thermotolerance, and transparent, which allows stable cycling of coin-type and flexible Li-air batteries under harsh conditions, such as a highly volatile DMSO electrolyte (over 660 h), a humid air (O 2 ) atmosphere (over 700 h) or circumstances in air (O 2 )-saturated liquid water (over 25 h). This work could potentially open a new research direction in developing O 2 -permeable membranes through hydrogen-bond cross-linking for the unfettered design of metal-air batteries.
研究领域:
材料科学
·
能源存储技术
✓ 已验证
产品关联
DOI
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.
研究领域:
催化化学
·
材料科学
·
理论计算化学
✓ 已验证
产品关联
DOI
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.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Xiangcheng Zhang,Jingzhen Zhang,Jie Miao,Xue Wen,Chao Chen,Baoxue Zhou,Mingce Long
Photocatalytic H 2 O 2 production is a promising strategy for decentralized applications, but to realize efficient H 2 O 2 production in the ambient conditions and absence of organic sacrifice remains challengeable. Herein, anthraquinone functionalized covalent organic frameworks (TpAQ-COFs) were fabricated by β-ketoenamines links of 2,6-diaminoanthraquinone (AQ) and 2, 4, 6-triformylphloroglucinol (Tp), and the structures and compositions were tuned by controlling the condensation time. The increase of time favors the assembly of TpAQ-COFs into more ordered lamellar stacking structure, and induces the increase of enol-imine form. The critical role of anthraquinone moieties as the active sites for oxygen reduction was proved, that is, facilitating charge separation and enhancing the activity and selectivity of H 2 O 2 production. Upon visible light irradiation, the TpAQ-COF synthesized after 12 h reaction has the highest content of anthraquinone moieties and the best performance for H 2 O 2 production (420 μmol h −1 g −1 ) in the absence of organic sacrificial agents. These findings bring insights to incorporate anthraquinone chemistry into photocatalysts at molecular levels for efficient H 2 O 2 production.
研究领域:
材料科学
·
环境科学
·
化学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）