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
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
SOLID STATE IONICS
·
2016
·
IF 2.38
Guofeng Xu,Qingrui Xue,Jianling Li,Zhanyu Li,Xinping Li,Tianheng Yu,Jiguang Li,Xindong Wang,Feiyu Kang
Lithium-excess layered cathode materials Li[Li 0.2 Mn 0.54 − x Sm x Co 0.13 Ni 0.13 ]O 2 (x = 0, 0.01, 0.03, 0.05) with different quantities of Sm were synthesized by the coprecipitation-calcination method. The rare earth element samarium (Sm) was introduced into the structure of Li[Li 0.2 Mn 0.54 Co 0.13 Ni 0.13 ]O 2 as the replacement at Mn sites. The refinement unit cell parameters from the X-ray powder diffraction patterns illustrate the doping of Sm facilitates enlarging the lithium ions diffusion passageway space of the Li[Li 0 . 2 Mn 0.54 Co 0 . 13 Ni 0.13 ]O 2 structure. The Li[Li 0.2 Mn 0.51 Sm 0.03 Co 0.13 Ni 0.13 ]O 2 electrode presented the best electrochemistry properties. The initial discharge capacity is 287.5 mAh g − 1 and the initial coulombic efficiency increases from 81.31% to 85.34% with a constant current density of 12.5 mA g − 1 , which can be attributed to the suppression of the oxygen release from the structure at the initial charge-discharge process. The Li[Li 0·2 Mn 0.51 Sm 0.03 Co 0.13 Ni 0.13 ]O 2 electrode delivers 236.1 mAh g − 1 after 40 cycles and the capacity retention ratio is 82.12% while only 206.8 mAh g − 1 and 70.85% are obtained after 40 times of cycling for the pristine electrode. The Nyquist plots indicate that the electrical conductivity and interfacial electrochemical reaction activity increase as well.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
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
·
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
MATERIALS LETTERS
·
2014
·
IF 2.269
Ming Yan,Yan Yan,Chao Wang,Wei Lu,Weidong Shi
In this letter, Ni 2+ doped InVO 4 nanocrystals were successfully synthesized by a simple one-pot microwave-assisted method. The energy bandgap of obtained samples can be precisely controlled by varying the Ni 2+ doping amount. The O 2 production rate of obtained Ni–InVO 4 nanocrystals is higher than that of pure InVO 4 nanocrystals under visible-light, which can be ascribed to the narrowed band gaps. The corresponding 1% doped sample N1 has the highest O 2 production rate (394 μmol/h) in all samples, which is 66% higher than the undoped sample N0.
研究领域:
材料科学
·
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
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.
研究领域:
癌症治疗
·
纳米技术
·
生物医学工程
·
药学
✓ 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
·
电化学
✓ 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
Nano Research
·
2023
·Vol. 16
·期 11
·12697-12705
·
IF 9.9
Gao Xinshuang,Zheng Jia-jia,Li Hanbo,Cai Rui,Gao Xingfa,Wu Xiaochun
Nanozymes, as a novel form of enzyme mimics, have garnered considerable interest. Despite overcoming the main disadvantages of their natural analogs, they still face challenges such as restricted mimic types and low substrate specificity. Herein, we introduce a reactive ligand modification strategy to diversify enzyme mimic types. Specifically, we have utilized helical plasmonic nanorods (HPNRs) modified with para -nitrothiophenol (4-NTP) to create an oxygen-sensitive nitroreductase (NTR) with light-controllability. HPNRs act as a light-adjustable source of nicotinamide adenine dinucleotide/nicotinamide adenine dinucleotide phosphate (NAD(P)H), providing photon-generated energetic electrons to adsorbed 4-NTP molecules. In the presence of O 2 , the activated 4-NTP transfers the captured electron to the adsorbed O 2 , mimicking the electron transfer process in its natural counterpart. This enhanced O 2 activation notably boosts the oxidative coupling of para -aminothiophenol (4-ATP). Density functional theory (DFT) calculations reveal that hot electrons injected into the lowest unoccupied molecular orbital (LUMO) energy level of 4-NTP can be transferred to that of molecular oxygen. In conclusion, our findings underline the potential of the reactive ligand modification strategy in developing new types of enzyme reactions, which opens up promising avenues for the enhancement and diversification of nanozyme functionalities.
研究领域:
生物化学
·
纳米生物学
·
催化科学
✓ 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）