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NEW JOURNAL OF CHEMISTRY · 2020 ·Vol. 44 ·期 27 ·11808-11816 · IF 3.288

Self-supported beaded Au@Co3O4 nanowire arrays perform electrocatalytic CO2 reduction in water to syngas and water oxidation to O2

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).

研究领域: 材料科学 · 电催化
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Journal of Materials Chemistry A · 2015 ·Vol. 4 ·期 4 ·1399-1407 · IF 7.443

A graphitic foam framework with hierarchical pore structure as self-supported electrodes of Li–O2 batteries and Li ion batteries

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).

研究领域: 材料科学 · 能源技术
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Journal of Materials Chemistry A · 2020 ·Vol. 8 ·期 19 ·9813-9824 · IF 11.301

The fabrication of IMo6@iPAF-1 as an enzyme mimic in heterogeneous catalysis for oxidative desulfurization under O2 or air

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.

研究领域: 化学 · 环境科学 · 材料科学
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JOURNAL OF HAZARDOUS MATERIALS · 2020 · IF 9.038

Catalytic activation of O2 by Al0-CNTs-Cu2O composite for Fenton-like degradation of sulfamerazine antibiotic at wide pH range

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 .

CAS / MDL: 7429-90-5 25322-68-3
研究领域: 环境科学 · 化学工程
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Nanoscale · 2019 ·Vol. 11 ·期 31 ·14654-14667 · IF 6.97

MnFe2O4-decorated large-pore mesoporous silica-coated upconversion nanoparticles for near-infrared light-induced and O2 self-sufficient photodynamic therapy

Binbin Ding,Shuai Shao,Haihua Xiao,Chunqiang Sun,Xuechao Cai,Fan Jiang,Xueyan Zhao,Ping'an Ma,Jun Lin

The limited light penetration depth and tumor hypoxia are two natural shortcomings of photodynamic therapy (PDT). Overcoming these two issues within a single system is still a great challenge. Herein, photosensitizer (PS)-loaded and PEG-modified MnFe2O4-decorated large-pore mesoporous silica-coated β-NaYF4:20%Yb,2%Er@β-NaYF4 upconversion nanoparticles (UCMnFe-PS-PEG) as excellent PDT agents are successfully prepared for NIR light-mediated and O2 self-sufficient PDT. The large mesoporous structure observably increases PS loading efficiency (11.33 wt%) and the green luminescence from upconversion nanoparticles activated by NIR is able to activate PSs to generate ROS effectively. In addition, sub-10 nm MnFe2O4 nanoparticles work as a Fenton catalyst to generate O2in situ. In vivo experiments further prove that UCMnFe-PS-PEG not only provides magnetic guidance to the tumor, but also overcomes tumor hypoxia and dramatically enhances PDT efficiency. Furthermore, in vivo MR and UCL imaging are performed for accurate cancer therapy. We believe that the successful construction of the multifunctional UCMnFe-PS-PEG provides more revelations for developing advanced nano-drug systems for cancer therapy.

研究领域: 生物医学工程 · 纳米医学 · 肿瘤治疗
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ACS Applied Bio Materials · 2023 · IF 4.7

O2-Generation-Enhanced Responsive Starvation/Photothermal Synergistic Tumor Therapy Based on the AuNRs@MnO2@SiO2 Nanocarrier and Thermosensitive Biomimetic Camouflaging

Wen-Xing Zhang,Ze-Lei Zhou,Qi-Yan Lv,Xiejie Song,Junyang Chen,Chang-Bin Niu,Hui-Fang Cui

Cancer starvation/photothermal combined tumor therapy (CST/PTT) has attracted great interest attributed to their mutual compensation and synergistically enhanced effect. However, the very low O2 supply in the tumor microenvironment (TME) greatly limits the CST efficiency of glucose oxidase (GOx). Additionally, the easy degradation in blood circulation and significant off-target effects are big challenges for clinical applications of the GOx-based CST. In this study, a drug delivery system (DDS) with specific tumor-targeted GOx delivery, near-infrared (NIR) light and TME responsive O2 generation, NIR-responsive glucose consumption, high GOx loading, and efficient NIR photothermia was developed. Positively charged AuNRs@MnO2@SiO2 nanoparticles (named AMS+ NPs) were synthesized. GOx was covalently loaded with a high loading ratio of 36.0%. Finally, a thermosensitive biomimetic hybrid membrane composed of a thermosensitive lipid (TSL) membrane, red blood cell membrane (RBCM), and 4T1 cancer cell membrane (CCM) was coated on the NPs through a double-layer strategy. The AMS+-G@TSL@[RBC-CC-TSL]M NPs consumed 32.7 times glucose at 50 °C as that at 37 °C and generated 4.9 times O2 upon NIR laser irradiation. The thermosensitive biomimetic NPs showed an efficient targeting capability to the homotypic 4T1 cancer cells/tumors accompanied by good biocompatibility, macrophage evading capability, high cancer cell cytotoxicity, and excellent antitumor efficacy. The tumor growth inhibition ratio with NIR laser irradiation reached 92.8%. The AMS+-GOx@TSL@[RBC-CC-TSL]M NPs provide a smart, efficient, safe, PTT/CST combined DDS for highly efficient tumor therapy.

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RARE METALS · 2023 ·Vol. 42 ·期 6 ·1969-1982 · IF 8.8

A ZnO decorated 3D copper foam as a lithiophilic host to construct composite lithium metal anodes for Li–O2 batteries

Liao Jia-Lin,Zhang Shuai,Bai Tian-Sheng,Ji Feng-Jun,Li De-Ping,Cheng Jun,Zhang Hong-Qiang,Lu Jing-Yu,Gao Quan,Ci Li-Jie

Lithium metal batteries (LMBs) with a high theoretical capacity are seen as a type of the most potential energy storage system. Unfortunately, the growth of lithium dendrite, the irreversible side reactions, and the infinite volume alteration still curb the practical utilization of lithium metal anodes, resulting in low Coulombic efficiency (CE) and safety problems, etc. Herein, we synthesize a lithiophilic 3D copper foam host with uniformly distributed nano-flower-like ZnO particles (CuF/ZnO) and obtain the composite lithium metal anode containing the Li 2 O, LiZn alloy, and pure Li by the infusion of molten Li (CuF/Li 2 O-LiZn@Li). Benefitting from the advantages of the 3D structure of copper foam and the lithiophilicity of ZnO sites, the composite lithium metal anode can restrain the volume alternation and regulate the uniform deposition of lithium. The symmetrical cells of the composite lithium metal anode have a 1600 h long cycle life with a low polarization voltage of 15 mV, and the Coulombic efficiency can maintain about 97.8% at 1.0 mA·cm −2 , 1.0 mAh·cm −2 . Graphical abstract

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Catalysts · 2023 ·Vol. 13 ·期 3 ·577 · IF 3.9

First Application of Nitrogen-Doped Carbon Nanosheets Derived from Lotus Leaves as the Electrode Catalyst for Li-CO2/O2 Battery

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

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Acta Biomaterialia · 2023 · IF 9.7

Hyaluronic acid-based supramolecular nanomedicine with optimized ratio of oxaliplatin/chlorin e6 for combined chemotherapy and O2-economized photodynamic therapy

Yuan-Fu Ding,Xun Xu,Junyan Li,Ziyi Wang,Jingwei Luo,Greta S.P. Mok,Shengke Li,Ruibing Wang

Dual- or multi-modality combination therapy has become one of the most effective strategies to overcome drug resistance in cancer therapy, and the optimized ratio of the therapeutic agents working on the tumor greatly affects the therapeutic outcomes. However, the absence of a facile method to optimize the ratio of therapeutic agents in nanomedicine has, at least in part, impaired the clinical potential of combination therapy. Herein, a new cucurbit[7]uril (CB[7])-conjugated hyaluronic acid (HA) based nanomedicine was developed, in which both chlorin e6 (Ce6) and oxaliplatin (OX) were co-loaded non-covalently at an optimized ratio via facile host-guest complexation, for optimal, combined photodynamic therapy (PDT)/chemotherapy. To maximize the therapeutic efficacy, a mitochondrial respiration inhibitor, atovaquone (Ato), was also loaded into the nanomedicine to limit consumption of oxygen by the solid tumor, sparing oxygen for more efficient PDT. Additionally, HA on the surface of nanomedicine allowed targeted delivery to cancer cells with over-expressed CD44 receptors (such as CT26 cell lines). Thus, this supramolecular nanomedicine platform with an optimal ratio of photosensitizer and chemotherapeutic agent not only provides an important new tool for enhanced PDT/chemotherapy of solid tumors, but also offers a CB[7]-based host-guest complexation strategy to facilely optimize the ratio of therapeutic agents for multi-modality nanomedicine. Statement of significance Chemotherapy remains the most common modality for cancer treatment in clinical practice. Combination therapy by co-delivery of two or more therapeutic agents has been recognized as one of the most effective strategies to improve therapeutic outcome of cancer treatment. However, the ratio of loaded drugs could not be facilely optimized, which may greatly affect the combination efficiency and overall therapeutic outcome. Herein, we developed a hyaluronic acid based supramolecular nanomedicine with facile method to optimize the ratio of two therapeutic agents for improved therapeutic outcome. This supramolecular nanomedicine not only provides an important new tool for enhanced photodynamic therapy/chemotherapy of solid tumors, but also offers insights in using macrocyclic molecule-based host-guest complexation to facilely optimize the ratio of therapeutic agents in multi-modality nanomedicine.

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Journal of Energy Chemistry · 2022 · IF 13.599

Superior oxygen electrocatalyst derived from metal organic coordination polymers by instantaneous nucleation and epitaxial growth for rechargeable Li-O2 battery

Dongdong Li,Jinbiao Chen,Yingtong Chen,Yian Wang,Yanpeng Fu,Minhua Shao,Zhicong Shi

Rechargeable aprotic Li-O 2 batteries have attracted increasing attention due to their extremely high capacity, and it is very important to design appropriate strategies to synthesize efficient catalysts used as oxygen cathode. In present work, we present an expedient “instantaneous nucleation and epitaxial growth” (INEG) synthesis strategy for convenient and large-scale synthesis of ultrafine MOCPs nanoparticles (size 50–100 nm) with obvious advantages such as fast synthesis, high yields, low costs and reduced synthetic steps. The bimetallic Ru/Co-MOCPs are further pyrolyzed to obtain bimetallic Co– and low content of Ru-based nanoparticles embedded within nitrogen-doped carbon (Ru/Co@N C) as an efficient catalyst used in Li-O 2 battery. The Ru/Co@N C provides porous carbon framework for the ion transportation and O 2 diffusion, and has large amounts of metal/nonmetal sites as active site to promote the oxygen reduction reaction (ORR)/oxygen evolution reaction (OER) in Li-O 2 batteries. As a consequence, a high discharge specific capacity of 15246 mA h g −1 at 250 mA g −1 , excellent rate capability at different current densities, and stable overpotential during cycling, are achieved. This work opened up a new understanding for the industrialized synthesis of ultrafine catalysts for Li-O 2 batteries with excellent structural characteristics and electrochemical performance.

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CERAMICS INTERNATIONAL · 2022 · IF 5.532

The effect of plasma-assisted ball milling on preparation and sintering behavior of (Zr0.1429Hf0.1429Ce0.1429Y0.2857La0.2857)O2-δ high entropy fluorite oxide

Chufei Cheng,Fengnian Zhang,Fuhao Cheng,Jiadong Hou,Bei Ren,Yang Miao,Libiao Xin,Xiaomin Wang

The sintering process of high entropy fluorite oxide ceramics prepared by the conventional solid-phase reaction method suffers from high single-phase synthesis temperature, low densities, and abnormal grain growth . To improve the sintering characteristics of high entropy fluorite oxide ceramics, the oxide mixture was dealt with dielectric barrier discharge plasma-assisted ball milling. The samples were analyzed using XRD , SEM, TEM, TG/DTG, visual high-temperature deformation analyzer, and nanoindentation meter. The results show that the plasma field activates the raw material powder and promotes powder finer. The rapid heating effect of the plasma during the ball milling process causes micro-area sintering and micro-area melting on the powder surface, which increases the active sites of the solid phase reaction of the material, accelerates the mass transfer process, and improves the sintering activity. Compared with conventional ball milling, plasma-assisted ball milling reduces the single-phase synthesis temperature of high entropy ceramics from 1500 °C to 1300 °C. The sintered ceramic pellets have intact grain growth, no noticeable abnormal grain growth, and improved density and mechanical properties .

CAS / MDL: 1306-38-3
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Carbon Energy · 2023 ·Vol. 5 ·期 8 ·e334 · IF 20.5

Double spatial confinement on ruthenium nanoparticles inside carbon frameworks as durable catalysts for a quasi-solid-state Li–O2 battery

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.

CAS / MDL: 10196-18-6
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