Joule
·
2022
·
IF 46.048
Qing Han,Wei Guo,Xiaofeng He,Tongchao Liu,Xiao Liu,Xuebing Zhu,Tengfei Bian,Lei Jiang,Jun Lu,Yong Zhao
Aprotic lithium-oxygen (Li-O 2 ) batteries have attracted extensive attention due to their ultrahigh theoretical energy density. However, slow and undesired electron transfer during cathodic reactions causes low cyclic stability in these batteries. Here, we demonstrate that O 2 mass transport and electron transfer for cathodic reactions in Li-O 2 batteries could be decoupled by a double-cathode structure that efficiently enables stable electron transfer between the cathode and Li 2 O 2 /O 2 . This resolves various side reactions and slow Li 2 O 2 reaction kinetics issues in conventional Li-O 2 batteries, leading to stable operation of the cell for nearly 2 months at a capacity of 0.2 and 5 mAh cm −2 , with more than 4- and 10-fold increases in cycle life when compared with single-cathode batteries. These remarkable improvements in the cyclic stability of Li-O 2 batteries with double cathodes provide an interesting concept for improving the operational stability of other metal-rechargeable batteries with conversion-type chemistry.
研究领域:
电化学
·
材料科学
·
能源存储
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DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2021
·Vol. 32
·期 15
·2111125
·
IF 18.808
Binyao Liu,Jinyan Du,Gaili Ke,Bi Jia,Yujie Huang,Huichao He,Yong Zhou,Zhigang Zou
g -C 3 N 4 photocatalysis is a safe and green approach for H 2 O 2 production, but the activity of pristine g -C 3 N 4 photocatalysts is unsatisfactory. At present, most of the modifications on g -C 3 N 4 photocatalysts for H 2 O 2 production have focused on thermodynamic processes, few have considered the kinetic aspects. Herein, the surface N -hydroxymethylation of g -C 3 N 4 photocatalysts for the efficient kinetic production of H 2 O 2 is reported. Through the reaction of formaldehyde with the amino moieties (–NH 2 ) on the g -C 3 N 4 surface, N -hydroxymethyls groups (-NH-CH 2 -OH) are introduced on typical g -C 3 N 4 photocatalysts. Relative to the pristine g -C 3 N 4 photocatalysts, the modified g -C 3 N 4 photocatalysts have over 1280% higher activity for H 2 O 2 production in pure water system, and impressive solar-to-chemical conversion efficiency. The experimental investigations and theoretical calculations reveal that the introduction of -NH-CH 2 -OH on the g -C 3 N 4 photocatalysts does not change their morphology, light absorption intensity and edges, band positions, charge separation and transfer properties, but markedly improved the H 2 O dehydrogenation and O 2 adsorption properties of g -C 3 N 4 . As a result, the reduction kinetics of O 2 to H 2 O 2 on the g -C 3 N 4 photocatalysts with -NH-CH 2 -OH is more energetically favorable. This work provides a useful reference and inspiration to achieve the effective modification of g -C 3 N 4 or other metal-free photocatalysts from the kinetic perspective.
研究领域:
光催化
·
材料科学
·
化学动力学
·
可再生能源
·
环境化学
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DOI
高影响因子
Science Bulletin
·
2025
·
IF 21.1
Ergui Luo,Jingyi Liang,Kexuan Zhang,Xian Wang,Luozhen Jiang,Tianjun Hu,Junming Zhang,Junjie Ge,Jianfeng Jia
Electrochemical two-electron oxygen reduction reaction (2e − ORR) serves as an appealing approach for green hydrogen peroxide (H 2 O 2 ) production. However, the corresponding progress in efficient non-precious metal catalysts for acidic 2e − ORR has not kept pace, with the research model being almost confined to Co-based system. Here, guided by molecular dynamics simulations, the active nature and origin of pyrolyzed Cr−N 4 catalysts for ORR are unveiled, wherein the over-strong oxygen affinity of the Cr center is counterbalanced by a spontaneous axial O-coordination. By creating an oxidation-induced electron-deficient environment, the Cr−N 4 can be flexibly tailored for selective H 2 O 2 formation. A single-atom Cr−N 4 /C(O) catalyst is developed experimentally, which rivals and even slightly outperforms its Co-based counterpart in terms of selectivity (92% versus 71%) and productivity (202 versus 145 mmol g cat −1 h −1 ) for H 2 O 2 . More encouragingly, the Cr-based catalysts exhibit minimal reactivity towards H 2 O 2 -related side reactions, with the metal component being robust against leaching. This research marks the first identification of pyrolyzed Cr−N 4 catalysts as competent for acidic two-electron O 2 reduction to H 2 O 2 . The innovative models and insights offer profound guidance for the design of future-generation catalysts for electrochemical H 2 O 2 synthesis.
研究领域:
电催化
·
材料科学
·
能源化学
·
可持续化学
·
计算化学
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产品关联
DOI
PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Shan Jiang,Jing Cao,Minna Guo,Dongdong Cao,Xuemei Jia,Haili Lin,Shifu Chen
Elemental red phosphorus (RP) has an ultra-low activity of splitting water for H 2 and O 2 evolution. In this study, RP was decorated by trace amount of WO 3 to greatly enhance the photocarriers separation and photocatalytic activity for overall water splitting under visible light. The 2.5% WO 3 /RP composite achieved the highest activity to produce H 2 and O 2 , and the activity was 7.0 times that of pure RP under visible light (λ ≥ 420 nm). The significantly increased photocarriers separation of WO 3 /RP was ensured by transient photocurrent, electrochemical impendence, photoluminescence, and time-resolved photoluminescence characterizations. More importantly, WO 3 /RP maintained high stability when it was persistently used for 20 cycles. Based on the reactive oxygen species ( O 2 − and OH) detected during the photocatalytic process, an S-scheme mechanism was proposed for WO 3 /RP composites to efficiently separate the photocarriers. This work provides a notion for improving the overall water splitting activity of RP via an S-scheme photocarriers separation mode.
研究领域:
材料科学
·
环境科学
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DOI
高影响因子
Materials Today Energy
·
2022
·
IF 9.257
Jingjun Zhai,Haocheng Ji,Wenhai Ji,Rui Wang,Zhongyuan Huang,Tingting Yang,Chaoqi Wang,Taolve Zhang,Ziwei Chen,Wenguang Zhao,Akhil Tayal,Lei Jin,Jun Wang,Yinguo Xiao
Layered transition metal oxides have been broadly studied due to their great potential in application as cathodes for sodium-ion batteries. However, many single-phase layered transition metal oxides, especially those crystallized in P2- or O3-type structure, possess their individual characteristics incurring unsatisfactory overall performances with respect to the reversible capacity, rate capability, and cycling stability. Here, an effective strategy of constructing the P2/O3 biphasic structure is realized in layered cathode Na 0.7 Ni 0.4 Mn 0.4 Ti 0.2 O 2 through Ti substitution. Through high-resolution scanning transmission electron microscopy and X-ray diffraction, the formation of P2/O3 intergrowth structure was clarified and the proportion of the two phases was determined. Benefitting from the presence of intergrowth structure, the layered cathode provides a competitive rate capability of 100 mAh/g at a high rate of 5 C as well as a prominent cycling stability of 80.04% capacity retention after 300 cycles at 5 C. The improved performance is closely related to the highly reversible phase transition process from P2/O3 to OP4/P3 with less strain and enhanced Na + kinetics. These findings evidence that exploring novel multiphase cathodes is an effective approach to improve the electrochemical performances of cathode for sodium-ion batteries.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
ACS Applied Bio Materials
·
2023
·
IF 4.7
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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产品关联
DOI
PubMed
高影响因子
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
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DOI
高影响因子
RARE METALS
·
2023
·Vol. 42
·期 6
·1969-1982
·
IF 8.8
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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产品关联
DOI
高影响因子
Acta Biomaterialia
·
2023
·
IF 9.7
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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产品关联
DOI
PubMed
高影响因子
Nanoscale
·
2019
·Vol. 11
·期 31
·14654-14667
·
IF 6.97
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.
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产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Shaomian Liu,Wenjuan Xue,Yongjun Ji,Wenqing Xu,Wenxing Chen,Lihua Jia,Tingyu Zhu,Ziyi Zhong,Guangwen Xu,Donghai Mei,Fabing Su
Simultaneously improving both NO x conversion and N 2 selectivity in the selective catalytic reduction of NO by CO (CO-SCR) under O 2 -containing conditions is highly challenging because of the competitive reactions of NO x and CO with O 2 . Here, we demonstrate that the interfacial oxygen vacancies (IOVs) generated at the Co 3 O 4 -CeO 2 heterointerfaces by ball-milling-induced strain can remarkably boost both NO x conversion and N 2 selectivity in the temperature range of 100–400 °C. The Co 3 O 4 -CeO 2 -IOV catalyst achieved approximately 100% NO x conversion and 100% N 2 selectivity (200–350 °C, 1–5 vol% O 2 , and 20,000 h −1 ); even under 10 vol% O 2 , it still showed good catalytic performance. The spectroscopy analysis and theoretical calculations reveal that compared with O 2 activation, IOVs are more favorable for the rate-limiting step of NO adsorption and dissociation. This work provides an effective strategy to create IOVs within metal oxide composite catalysts using ball-milling-induced interfacial strain for improving CO-SCR performance.
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产品关联
DOI
高影响因子
Journal of Advanced Ceramics
·
2022
·Vol. 11
·期 11
·1801-1814
·
IF 11.534
Cheng Fuhao,Zhang Fengnian,Liu Yufeng,Guo Meng,Cheng Chufei,Hou Jiadong,Miao Yang,Gao Feng,Wang Xiaomin
Environmental barrier coatings (EBCs) with excellent chemical resistance and good high-temperature stability are of great significance for their applications in next-generation turbine engines. In this work, a new type of high-entropy fluorite-structured oxide (Ce 0.2 Hf 0.2 Y 0.2 Pr 0.2 Gd 0.2 )O 2− δ (HEFO-1) with different Ti 4+ contents were successfully synthesized. Minor addition of Ti 4+ could be dissolved into a high-entropy lattice to maintain the structure stable, effectively reducing the phase formation temperature and promoting the shrinkage of bulk samples. Heat treatment experiments showed that all the samples remained a single phase after annealing at 1200–1600 °C for 6 h. In addition, high-entropy (Ce 0.2 Hf 0.2 Y 0.2 Pr 0.2 Gd 0.2 Ti 0.2 x )O 2− δ demonstrated great resistance to calcium—magnesium—alumina—silicate (CMAS) thermochemical corrosion. When the content of Ti was increased to x = 0.5, the average thickness of the reaction layer was about 10.5 after being corroded at 1300 °C for 10 h. This study reveals that high-entropy (Ce 0.2 Hf 0.2 Y 0.2 Pr 0.2 Gd 0.2 Ti 0.2 x )O 2− δ is expected to be a candidate for the next-generation EBC materials with graceful resistance to CMAS corrosion.
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）