Catalysts
·
2023
·Vol. 13
·期 3
·577
·
IF 3.9
Lu Zou,Weilin Kong,Linfeng Peng,Fang Wang
The development of Li-CO2/O2battery with high energy density and long-term stability is urgently needed to fulfill the carbon neutralization and pollution-free environment targets. The biomass-derived heteroatom-doped carbon catalyst with the combination of high-efficiency catalytic activity and sustainable supply is a promising cathode catalyst in Li-CO2/O2battery. Specifically, the unique morphology and mesopore structure can promote the transfer of CO2, O2, and Li+. Abundant channel pores can provide discharge products accommodation to the largest extent. Nitrogen dopant, the commonly recognized active sites in carbon, can improve the electron conductivity and accelerate the sluggish kinetic reaction. Therefore, utilizing the louts leaves as the precursor, we successfully prepare the cellular-like nitrogen-doped activated carbon nanosheets (N-CNs) through the appropriate pyrolysis carbonization method. The as-synthesized carbon nanosheets display a three-dimensional interconnecting pore structure and abundant N-dopant actives, which dramatically improve the electrochemical catalytic activity of N-CNs. The Li-CO2/O2battery with the N-CNs cathode delivers a high discharge capacity of 9825 mAh g−1, low overpotential of 1.21 V, and stable cycling performance of 95 cycles. Thus, we carry out a facile method for N-doped carbon nanosheets preparation derived from the cheap natural biomass, which can be the effective cathode catalyst for environmental-friendly Li-CO2/O2battery.Keywords:biomass-derived carbon;carbon nanosheets;nitrogen defects;cathode catalyst;Li-CO2/O2battery
研究领域:
材料科学
·
环境科学
·
能源科学
✓ 已验证
DOI
高影响因子
Carbon Energy
·
2023
·Vol. 5
·期 8
·e334
·
IF 20.5
Meiling Wang,Ying Yao,Feiyang Yang,Zhenwu Tang,Jingjie Ren,Cunzhong Zhang,Feng Wu,Xiangke Wang
The rational design of large-area exposure, nonagglomeration, and long-range dispersion of metal nanoparticles (NPs) in the catalysts is critical for the development of energy storage and conversion systems. Little attention has been focused on modulating and developing catalyst interface contact engineering between a carbon substrate and dispersed metal. Here, a highly dispersed ultrafine ruthenium (Ru) NP strategy by double spatial confinement is proposed, that is, incorporating directed growth of metal–organic framework crystals into a bacterial cellulose templating substrate to integrate their respective merits as an excellent electrocatalytic cathode catalyst for a quasi-solid-state Li–O 2 battery. The porous carbon matrix with highly dispersed ultrafine Ru NPs is well designed and used as cathode catalysts in a Li–O 2 battery, demonstrating a high discharge areal capacity of 6.82 mAh cm –2 at 0.02 mA cm –2 , a high-rate capability of 4.93 mAh cm –2 at 0.2 mA cm –2 , and stable discharge/charge cycling for up to 500 cycles (2000 h) with low overpotentials of ~1.4 V. This fundamental understanding of the structure–performance relationship demonstrates a new and promising approach to optimize highly efficient cathode catalysts for solid-state Li–O 2 batteries.
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
Journal of Energy Storage
·
2022
·
IF 8.907
De-Ming Zhu,Fan Bai,Yi-Nan Zhang,Ya-Nan Yang,Zhuang Sun,Jun-Wen Deng,Tao Zhang
Solid-state Li-O 2 batteries (SSLOBs) have been denoted as the holy grail in next-generation Li metal batteries for their high theoretical energy density , manipulation of ambient air to energy storage as well as high safety. However, the solid rigid interfaces both at the cathode and anode side introduce ultra-high resistances in the battery system and impede its operation under ambient temperature. Moreover, the high-reductive Li anode and semi-open cathode would cause severe side reactions during cycling which further degrade battery performance. To manage the above-mentioned issues, a rationally designed SSLOBs based on plastic crystal electrolyte is proposed in this study to enable SSLOBs operation at ambient temperature and in full charge-discharge mode. The brand-new Li-O 2 battery has been improved mainly from two aspects. First, we propose a polyacrylonitrile (PAN) modified succinonitrile (SN) electrolyte (PAN-SN) to retard the polymerization of SN and meanwhile suppress the degradation of Li ionic conductivity. Second, we propose an alternative mixed electron/ion complex conductor (MEIC) cathode to coordinate with plastic crystal electrolyte with an expanded Li-O 2 reactive zone and improved interfacial charge transfer during the charge-discharge process. The fabricated flexible SSLOBs based on PAN-SN electrolyte and MEIC cathode could be successfully fully charged-discharged (cutoff 2.0–4.5 V) for tens of cycles at ambient temperature under simulated air condition (20 vol% oxygen), with high-capacity retention of around 85 %.
研究领域:
能源存储
·
电池技术
·
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2018
·
IF 6.653
Yuan Chen,Xu Zhang,Shixiang Feng
Contributions of excited triplet state of humic acid (3HA*) and superoxide radical anion (O2•–), which is mainly generated via the reaction of O2 with HA-derived reducing intermediates (HA•–), to phenol transformation were revealed using acetaminophen, 2,4,6-trimethylphenol and tyrosine as probe molecules. Phenol transformation was initiated by 3HA*, leading to the formation of the phenoxyl radical (PhO•), but the distribution of transformation intermediates was codetermined by 3HA* and HA•–. The influence of HA•– essentially resulted from the production of O2•–, which affected the fate of PhO•. PhO• could undergo dimerization, or react with O2•–, leading to either phenol peroxide formation (radical addition) or phenol regeneration (electron transfer). In addition, PhO• could bind to HA or react with HA radicals, particularly in the absence of O2 and O2•–. These PhO• reactions were dependent on the reduction potential and structure of PhO•. This study also proved that the reaction of phenol with 1O2 and the reaction of PhO• with O2•– lead to the same oxidation product. The contributions of 3HA* and its generated 1O2, HA•– and its generated O2•– to phenol transformation were pH-dependent.
研究领域:
环境化学
·
物理化学
·
分析化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·Vol. 30
·期 18
·53355-53369
·
IF 5.8
Ding Chunsheng,Lei Jia,Cai Zhiyue,Gao Mengying,Zou Zhaozheng,Li Yuanfeng,Deng Jing
In this research, FeCo 2 O 4 nanomaterial was successfully synthesized by a typical sol–gel method and conducted as an effective agent for peroxymonosulfate (PMS) activation to eliminate antibiotics flurbiprofen (FLU), a strong nonsteroidal drug. FeCo 2 O 4 nanomaterial was characterized by XRD, TEM, SEM, and XPS. Various characterization results proved that FeCo 2 O 4 held stable spinel structure. The interfering factors including initial pH, PMS concentration, catalyst dosage, inorganic anions, and humic acid on FLU removal were also discussed. The conclusion was that the removal efficiency of FLU reached 98.2% within 120 min after adding FeCo 2 O 4 (0.4 g L −1 ) and PMS (3 mM). The optimal pH for FLU degradation was the initial pH of 6.5; too acidic or alkaline was not conductive to the degradation. The existence of HA and Cl − restrained the degradation of FLU, and HCO 3 − promoted the removal, while the influence of NO 3 − and SO 4 2− could not be considered. The radical scavenging experiment confirmed that • OH, O 2 •− , and SO 4 •− participated in FLU removal and SO 4 •− functioned a leading role. FeCo 2 O 4 showed high efficiency for PMS activation in pH range of 3.0 to 10.0. After the fourth cycle operation, the FLU removal rate exceeded 76.9%, and the Co leaching rate was low during the catalytic reaction. This study shows that FeCo 2 O 4 nanomaterial is an efficient and environment-friendly catalyst, which can be applied for PMS activation to remove organic pollutants in water.
研究领域:
环境科学
·
化学
·
材料科学
·
水处理
✓ 已验证
产品关联
DOI
PubMed
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2023
·
IF 5.2
Geng Li,Zhuoyu Cai,Kun Su,Yuxin Zhao,Ying Zhu,Jiangang Han,Yuwei Pan,Weinan Xing,Guangyu Wu
In recent years, advanced oxidation technologies employ peroxynitrite activation have exhibited exceptional effectiveness in eliminating various emerging contaminants. In this study, different calcination temperatures were used to derive Co 3 O 4 nanospheres with varying surface morphologies . This method effectively addresses the issue of high cost associated with high-performance catalyst synthesis or poor catalytic performance of low-cost catalysts. The active species like O 2 •− , •OH, SO 4 •− , 1 O 2 played significant role in TC degradation and 1 O 2 was the dominant reactive oxygen species (ROS). The study also proposed possible degradation pathways based on the 15 intermediates identified through HPLC-MS. Furthermore, the developmental toxicity of the identified intermediates was evaluated using a quantitative conformational relationship prediction method. This paper delves into the reaction mechanism of Co 3 O 4 nanospheres in the activation of PMS and examines the impact of surface morphology on their catalytic performance, providing a new approach to developing a persulfate catalyst that is cost-effective and has high catalytic performance, with a simple synthesis step.
研究领域:
环境科学
·
化学工程
·
材料科学
·
高级氧化技术
·
催化
✓ 已验证
产品关联
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2023
·Vol. 34
·期 2
·2305470
·
IF 19
Hangyu Lu,Shiyong Chu,Jiaming Tian,Qi Wang,Chuanchao Sheng,Chen Cheng,Rixin Liu,Anita M. D'Angelo,Wei Kong Pang,Liang Zhang,Haoshen Zhou,Shaohua Guo
Lattice-oxygen redox in layered metal oxide cathodes offers a promising way to exploit high-energy density sodium-ion batteries. However, oxidation and reduction of lattice-oxygen are always asymmetric, showing poor reversibility upon charging and discharging due to the activated oxygen loss and subsequent structural rearrangement. Here, a layered Na 0.7 [Li 0.2 Mn 0.7 Co 0.1 ]O 2 (NLMCO) is developed by balancing lattice-oxygen activity and reversibility, which can deliver a record energy density of 729.7 Wh kg −1 , further exceeding the state-of-the-art Na 0.75 [Li 0.25 Mn 0.75 ]O 2 (NLMO, 638.4 Wh kg −1 ). In light of electron paramagnetic resonance spectroscopy, in situ differential electrochemical mass spectroscopy, and electrochemical testing results, the highly activated lattice-oxygen is effectively stabilized in NLMCO without oxygen molecule release while obvious oxygen release is detected in the highly activated NLMO. Benefiting from the enhanced transition metal-oxygen covalency and reduced band energy gap, the NLMCO electrode demonstrates simultaneously high lattice-oxygen activity and reversibility, thus resulting in excellent rate and cycling performance, as well as ultra-high energy density. The findings highlight the critical association of energy density and lattice-oxygen redox reversibility, which will inspire more interest in anionic redox-based high-energy batteries.
研究领域:
材料科学
·
电池技术
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Liying Hao,Jikui Sun,Qingyin Wang,Haijiao Xie,Xiangui Yang,Qiang Wei
As an atom-economical reaction, the direct generation of dimethyl carbonate (DMC) and ethylene glycol (EG) via the transesterification of CH3OH and ethylene carbonate (EC) has several promising applications, but the exploration of carriers with high specific surface areas and novel heterogeneous catalysts with more basic sites remains a long-standing research challenge. For this purpose, herein, a nitrogen-doped mesoporous carbon (NMC, 439 m2/g) based K–O2 Lewis base catalyst (K–O2/NMC) with well-dispersed strongly basic sites (2.23 mmol/g, 84.5%) was designed and synthesized. The compositions and structures of NMC and K–O2/NMC were comprehensively investigated via Fourier transform infrared spectroscopy, X-ray diffraction, X-ray photoelectron spectroscopy, scanning electron microscopy, transmission electron microscopy, N2 adsorption–desorption, CO2 temperature-programmed desorption, and contact angle measurements. The optimal structural configuration and electron cloud distribution of the K–O2/NMC catalyst were simulated using first-principles calculations. The electron transfer predominantly manifested as a flow from K–O to C–O/C–N, and the interatomic interactions between each atom were enhanced and exhibited a tendency for a more stable state after redistribution. Furthermore, the adsorption energies (Eads) of CH3OH at K–O–O and K–O–N sites were −1.4185 eV and −1.3377 eV, respectively, and the O atom in CH3OH exhibited a stronger adsorption tendency for the K atom at the K–O–O site. Under the optimal conditions, the EC conversion, DMC/EG selectivity, and turnover number/frequency were 80.9%, 98.6%/99.4%, and 40.5/60.8 h–1, respectively, with a reaction rate constant (k) of 0.1005 mol/(L·min). Results showed that the heterogeneous K–O2/NMC catalyst prepared herein greatly reduced the reaction cost while guaranteeing the catalytic effect, and the whole system required a lower reaction temperature (65 °C), a shorter reaction time (40 min), and a lower catalyst amount (2.0 wt % of EC). Therefore, K–O2/NMC can be used as a catalyst in different transesterification reactions.
研究领域:
催化化学
·
材料科学
·
绿色化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Catalysis Science & Technology
·
2024
·
IF 4.4
Renjie Deng,Huajie Liu,Haishuai Cui,Yao Tian,Hai Yang
In this work, we have developed a green method for the preparation of para-nitrotoluene through the catalytic nitration of toluene with nitrogen dioxide (NO2) under the promotion of dioxygen (O2). The experimental results reveal that the dealumination of Hβ zeolite has a significant effect on the catalysis of the developed NO2–O2–acetic anhydride (Ac2O) system, in which the conversion of toluene is 78.1% and the selectivity to para-nitrotoluene is 71.8%. Furthermore, the nature of different dealuminated catalysts was investigated by nitrogen adsorption–desorption analysis, X-ray diffraction (XRD), Fourier-transform infrared (FT-IR), thermal gravimetric analysis (TGA), inductively coupled plasma (ICP), ammonia temperature-programmed desorption (NH3-TPD), pyridine adsorbed Fourier-transform infrared (Py-FT-IR), scanning electron microscopy (SEM) and 27Al magic-angle spinning nuclear magnetic resonance (27Al MAS NMR) techniques. The results of characterization indicate that the structure of the Hβ zeolite still remains and that of Al species in the extra-framework is preferentially removed after acid treatment. Based on the combined results of catalytic characterization and DFT calculation, a feasible reaction mechanism of improved para-selectivity in toluene nitration was suggested for the NO2–O2–Ac2O system.
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Leilei Hou,Siyang Yan,Liping Liu,Jiaxu Liu,Guang Xiong
The TS-1 microsphere was facilely prepared via a direct spray drying of the mixture containing the nanocrystal TS-1 and mother liquor. The calcined TS-1 zeolites possess a hollow structure and numerous intercrystalline mesopores, which may facilitate the diffusion properties. Au nanoparticles were loaded on TS-1 support by utilizing a deposition–precipitation process to prepare the Au/TS-1-M catalysts for propylene epoxidation in the presence of H 2 and O 2 conditions. The effects of the Ti and Au loadings on the structure, porosity, morphology, and catalytic performances of the Au/TS-1 catalysts have been investigated by various techniques. Under the optimized synthesis conditions (Si/Ti molar ratio = 57, 0.49 wt% Au), a propylene conversion of 6.1 % and a PO selectivity of 91.7 % were obtained on the Au/TS-1 catalyst. A PO formation rate of 186.8 g PO ·kg cat. −1 ·h −1 was achieved at the 20th hour.
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
ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Yang Zhan,Shun-zhi Yu,Shao-hua Luo,Jian Feng,Qing Wang
Transition-metal sulfides (TMS) are one of the most promising cathode catalysts for Li–O2 batteries (LOBs) owing to their excellent stabilities and inherent metallicity. In this work, a highly efficient mode has been used to synthesize Co@CNTs [pyrolysis products of metal–organic frameworks (MOFs)]-derived CoS2(CoS)@NC. Benefiting from the special yolk–shell hierarchical porous morphology, the existence of Co–N bonds, and dual-function catalytic activity (ORR/OER) of the open metal sites contributed by MOFs, the CoS2@NC-400/AB electrode illustrated excellent charge–discharge cycling for up to nearly 100 times at a current density of 0.1 mA cm–2 under a limited capacity of 500 mA h g–1 (based on the total weight of CoS2@NC and AB) with a high discharge voltage plateau and a low charge cut-off voltage. Meanwhile, the average transferred electron number (n) is around 3.7 per O2 molecule for CoS2@NC-400, which is the chief approach for a four-electron pathway of the ORR under alkaline media. Therefore, we believe that the novel CoS2@NC-400/AB electrode could serve as an excellent catalyst in the LOBs.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
PubMed
高影响因子
Small Methods
·
2022
·Vol. 6
·期 6
·2200178
·
IF 15.367
Rui Xu,Phei Er Saw,Lei Xu
Two-dimensional (2D) nanomaterials have attracted increasing attention in cancer theranostics due to their ultrahigh specific surface area resulting in more radicals and/or reactive oxygen species (ROS) generation in chemodynamic therapy (CDT). However, their biomedical prospects are greatly limited by poor biocompatibility, low dispersion, weak stability, and the potential threat of their high immunogenicity. Moreover, rapid depletion of ROS by the high level of antioxidants (e.g., glutathione) in cancer cells severely limits the therapeutic effects of cancer CDT. Herein, a robust method is developed to improve the biomedical application of 2D nanomaterials via constructing a 2D nanomaterials delivery nanoplatform with hemoglobin-based minerals biological coat for the safe encapsulation, long blood circulation, and controlled release of 2D nanomaterials. After intravenous administration and then internalization by cancer cells, the acidic microenvironment and high concentration of H 2 O 2 can trigger rapid release of Cu-T nanoscale metal-organic frameworks (nMOFs) from Cu-T@MH. Then, the released Cu-T nMOFs with simultaneous high ROS production and GSH depletion endow the Cu-T@MH nanoplatform with enhanced cancer CDT. Besides, the fluorescence recovery of tetrakis(4-carboxyphenyl) porphyrin in Cu-T nMOFs during the GSH depletion process can accurately visualize the cancer therapeutic action.
研究领域:
生物医学工程
·
肿瘤学
·
纳米医学
✓ 已验证
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）