Nano Energy
·
2021
·
IF 17.881
Dewang Li,Xiuyao Lang,Yong Guo,Yiqiao Wang,Yanyin Wang,Hucheng Shi,Shichao Wu,Weichao Wang,Quan-Hong Yang
Li-O 2 batteries are one of the most promising next generation batteries due to their high energy density . However, they suffer from high charge overpotentials and severe side reactions. Here we report a bifunctional CeVO 4 catalyst that not only lowers the charge potential by a photo-assisted mechanism, more importantly, promotes the efficient conversion of highly reactive oxidative intermediates to Li 2 O 2 , thus avoiding the oxidative decomposition of the electrolyte/cathode during discharge. Benefiting from its efficient electrocatalysis and the improved charging ability, 1.6x higher discharge capacity up to 6.14 mAh cm -2 , low charge potential of 3.48 V and stable cycling performance are simultaneously achieved. Theoretical calculation and in-situ Raman spectra confirm the superior adsorptive and conversion ability of superoxide species by electrochemical reduction and chemical disproportionation reactions on the CeVO 4 catalyst. These results indicate an effective strategy to break through the reported limitations of photo-assisted cathodes that are of a low electrocatalysis ability and limited discharge capacity. The significance of retaining a high energy density in photo-assisted Li-O 2 batteries is highlighted.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
·
IF 19.503
Qian Zhang,Yuanyu Shi,Xianjin Shi,Tingting Huang,Shuncheng Lee,Yu Huang,Jun-ji Cao
Photo-oxidative NO x removal often encountered with sluggish charge carrier separation kinetics and poor selectivity. Herein, Pd/ferroelectric Bi 4 Ti 3 O 12 nanoflakes (Pd/BTO NF) were constructed to investigate the photo-excited charge separation, O 2 activation and the generated reactive oxygen species (ROS) in dictating NO removal. Results showed that the depolarization field of ferroelectric BTO NF significantly promoted bulk charge separation, leading to boosted NO removal reaction kinetics (10 times higher) for Pd/BTO NF comparing with Pd/TiO 2 . Revealed by electronic paramagnetic resonance and radical scavenging tests, it is observed that the primary O 2 activation species differed among Pd, Ag and Pt supported BTO NF photocatalysts, which resulted in different selectivity. The underlying mechanism of NO photo-oxidative conversion pathway was studied by in situ diffuse reflectance infrared Fourier transform spectroscopy. This work illustrate that metal/ferroelectric interfaces can be tuned to obtain differing O 2 activation species, and notable selectivity changes in photocatalysis mediated environmental remediation reactions.
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Zichen Song,Xinxin Zhang,Jianqiu Zhu,Xiaolei Wang,Wenqian Wang,Xiangbo Ma,Jiantao Fu,Jian-Qiang Wang,Guiling Wang,Zhiyu Ren,Honggang Fu
While copper complexes intrinsically provide Cu sites for electrocatalytic CO 2 reduction (ECR), their efficacy toward multicarbon products (C 2+ ) remains fundamentally limited by the operational instability of reactive Cu valence states and the inability to synchronously optimize *CO intermediate generation and C-C coupling within symmetric coordination environments. Herein, we judiciously design a single-crystal N, O co-coordinated copper complex (Cu(ICA) 2 ) featuring asymmetric N 2 -Cu-O 2 centers that precisely modulate the electronic structure and local adsorption environment. The Cu-N bonds stabilize partially reduced Cu δ⁺ sites while weakening Cu-O interactions, thus balancing structural integrity with catalytic reactivity. This asymmetric dual-site coordination concurrently hosts distinct *CO intermediates (atop-adsorbed *CO at Cu sites and bridge-adsorbed *CO at Cu-N sites), enabling cooperative C-C coupling into C 2 products. The catalyst achieves a record 69.2 % Faradaic efficiency for C 2 products at 400 mA cm −2 and 57.4 % for C 2 H 4 at 500 mA cm −2 in 1.0 M KOH, rivaling the state-of-the-art Cu-based complexes. In situ characterization and DFT calculations mechanistically corroborate that bridge-adsorbed *CO at Cu-N sites drives energetically favorable hydrogenation and C-C coupling pathways. This work establishes a coordination-asymmetry design principle for constructing robust molecular catalysts capable of efficient CO 2 -to-C 2+ conversion.
研究领域:
电化学
·
催化化学
·
分子设计
·
能源材料
·
环境化学
·
物理化学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Zhen Wang,Lei Ying,Weibin Xu,Beien Zhu,Chuande Huang,Pengfei Wu,Qingqing Gu,Bing Yang,Jian Lin,Yi Gao,Xiaodong Wang,Tao Zhang
Tuning metal size from nanoscale to uniform single atoms holds the potential to promote the oxygenates selectivity for direct methane conversion, but suffers from low kinetics when utilizing O 2 as oxidant. Herein, we report a Au nano -Fe 1 -ZSM-5 catalyst for enhanced acetic acid production from CH 4 , CO, and O 2 in aqueous solution. The Au nano nanoparticles enable upgrading of O 2 into active hydroxyl radicals (•OH) via net reaction between O 2 , H 2 O and CO. The Fe 1 single atoms within 5-nm range from Au nano could be converted into active Fe 1 IV -O by •OH oxidation, which catalyzes rapid H-abstraction from CH 4 and subsequent C-C coupling with CO for acetic acid production. Such closely adjacent but separate active centers, i.e., Au nano and Fe 1 for decoupled O 2 and CH 4 activation, respectively, enable a high reactivity of 982 mmol/g metal /h for methane conversion with O 2 oxidant while retaining a high acetic acid selectivity of 81 % at 150 °C.
研究领域:
催化化学
·
能源化学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2024
·
IF 7.1
Zejia Wu,Jiashu Yuan,Hui Wang,Zaifa Pan,Jie Gao,Yonggao Xia
With the wide application of ternary lithium-ion batteries, the increased usage of batteries has resulted in a corresponding rise in the amount of discarded batteries. Here, we propose an efficient and prioritized lithium extraction process with a low environmental impact for the recovery of valuable metal components from spent LiNi0.5Co0.2Mn0.3O2 cathode materials. SO2 calcination–water leaching was used to recover Li, while H2SO4 acid leaching facilitated the recovery of Ni, Co, and Mn, yielding a precursor solution for the treatment of discarded NCM batteries. The effects of calcination temperature, calcination time, water leaching time, water leaching liquid–solid ratio, different battery ratios, acid leaching time, acid leaching liquid–solid ratio, and acid leaching temperature were optimized. The acid leaching process was controlled by surface chemical reactions through kinetic analysis. Under optimal conditions, Li was converted to soluble Li2SO4, achieving an impressive leaching rate of 99.7%. Ni, CO, and Mn were converted to their respective oxides. Furthermore, it was demonstrated that the formation of Li2Mn(SO4)2 from Mn with Li during calcination enhances the leaching efficiency across different battery composition ratios. The activation energies of Ni, Co, and Mn during the acid leaching process were determined by kinetic calculations, yielding values of 130.19, 133.05, and 134.09 kJ mol–1, respectively. This study provides a novel method for recycling spent NCM cathode materials.
研究领域:
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF POWER SOURCES
·
2024
·
IF 8.1
Yajun Zhao,Ke Meng,Teng Luo,Mengxu Chen,Shuai Niu,Cong Lin,Xianjun Xing,QinChun Yang,Xianghua Kong,Dawei Zhang,Hao Luo
The significant challenge faced by Li–O 2 batteries (LOBs) lies in their slow oxygen reduction and evolution kinetics, which greatly necessitates the development of highly active catalysts. Herein, we report a high-performance oxygen cathode (RuCo-NC) that is achieved by uniformly dispersing the nanoalloy of noble metal Ru and transition metal Co on the three-dimensional (3D) nanoporous carbon. Density functional theory (DFT) calculations reveal a prominent electron transfer process between Ru and Co, along with a substantial abundance of electron transfer sites on RuCo-NC. These characteristics contribute to a strong positive equilibrium effect on the formation and decomposition of Li 2 O 2 , which is crucial for LOBs. Furthermore, the calculated Gibbs free energy change during the oxygen reduction and evolution processes indicates that RuCo-NC exhibits the smallest overpotential compared to single metal catalysts . As a result, this RuCo-NC cathode enables the resulting LOB with a larger discharge specific capacity, lower overpotential for efficient oxygen reduction and evolution, and excellent cycling stability. This work introduces an effective method for fabricating nanoalloy catalysts with enhanced efficiency, promising advancements in energy applications .
研究领域:
材料科学
·
电化学
·
能源存储与转换
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Bohua Li,Jingning Lai,Fengling Zhang,Wen Sun,Zhengqiang Hu,Boshun Gui,Nan Chen,Li Li,Feng Wu,Renjie Chen
LiI in Li-O 2 batteries has shown promise in reducing charge overpotential. However, the shuttle effect of oxidated iodine species (OISs) can lead to lithium metal corrosion and loss of OISs. During the discharging process, these iodine species can undergo side reactions, resulting in the accumulation of LiOH and other parasitic products, which in turn accelerates battery failure. In this work, we have drawn inspiration from mussel protein and utilized a simple co-deposition method to form a robust biomimetic functionalized coating on the surface of the glass fiber separator. This was achieved by grafting catechol/polyamine (CA/PA) with 11-mercaptoundecanoic acid (MUA). This separator exhibits strong electrostatic repulsion towards negatively charged OISs and, conversely, electrostatic attraction towards Li + , this dual action effectively suppresses the shuttle effect and facilitates Li + transport. When equipped with this modified separator, the Li-O 2 battery effectively reduces the accumulation of LiOH and demonstrates significantly enhanced rate performance and cycle stability. Our findings provide a versatile approach for the design of modified separators for Li-O 2 batteries with redox mediators (RMs).
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
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Dan Li,Fu Sun,Yuqing Zhang,Yulong Liu,Hao Sun,Haiming Xie,Jia Liu,Seung-Taek Myung,Jiefang Zhu
In situ characterization on interface stability has been hardly tried in redox mediator (RM)-involved Li-O 2 battery thus far. Here, benzyltriethylammonium iodide (BTEAI) can act as a self-defensive RM in the electrolyte LiTFSI/TEGDME to enhance the reaction kinetics and increase the cycling stability by suppressing the redox shuttling. I - effectively reduces the charging overpotential by changing decomposition route for Li 2 O 2. BTEA + can facilitate LiTFSI decomposition in the electrolyte, and participate in formation of an organic–inorganic composite SEI-contained layer on Li anode. Moreover, for the first time, non-destructive synchrotron X-Ray tomography is used to investigate the mechanism of suppressing shuttle effect by monitoring the morphological evolution of electrodes interface. This work provides an insight into the development of functional RM and in situ protection strategies for Li anodes in Li-O 2 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
高影响因子
SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
·
2024
·
IF 4.3
Zhe Li,Xiaohui Wang,Xiuli Fu,Jinhua Liu,Yuanan Liu,Hongxin Zhang
The pH and O 2 are the two important parameters to evaluate environmental conditions, healthcare, and industrial processes. Herein, we developed a ratiometric fluorescent capillary-based dual-functional sensor for simultaneous monitoring of pH and O 2 fluctuations. The fluorescent sensor consists of a pH sensing unit and an O 2 sensing unit on both ends of the capillary inner wall. The ratiometric fluorescent pH sensing unit includes pH-sensitive probe HPTS and the reference dye Ce6, while the O 2 sensing unit is composed of O 2 -sensitive probe RuDP and the reference dye C6. Under single-wavelength excitation at 430 nm, the ratiometric fluorescent dual-functional sensor exhibits highly sensitive, selective and reproducible responses to both pH and O 2 . As for practical aqueous samples, the results about pH and O 2 levels obtained by our sensor are considerable consistent with commercial devices. Meanwhile, the dynamic changes of pH and O 2 levels during glucose catalysis by glucose oxidase can be detected in real-time and accurately. The dual-functional ratiometric fluorescent capillary transducer provides a significant potential platform for environmental monitoring and medical diagnosis.
研究领域:
生物医学工程
·
环境科学
·
化学传感
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Materials Research and Technology-JMR&T
·
2024
·
IF 6.2
Bo Ma,Zhiqin Wen,Jiedong Qin,Taoyi Lu,Li Tang,Zhenyu Wu,Yuhong Zhao
In this paper, in order to improve the mechanical properties of high-entropy fluorite oxides (HEFOs), five equimolar multicomponent oxides were synthesized by solid-phase reaction method by using element Y replacing one of the five cations in (Ce 0.2 Zr 0.2 La 0.2 Sm 0.2 Nd 0.2 )O 2- δ . The substitution of La, Sm or Nd in (Ce 0.2 Zr 0.2 La 0.2 Sm 0.2 Nd 0.2 )O 2- δ with Y element are able to form single-phase HEFOs at 1600 °C, while Ce 4+ and Zr 4+ replaced by Y 3+ contains a large number of secondary phase. The former three components are almost dense and smooth, and all the elements are uniformly distributed with no obvious segregation and agglomeration. The Ce 3+ concentration of Y-substituted Sm HEFOs is calculated to be 13.7%, yielding a nominal composition of (Ce 0.2 Zr 0.2 Y 0.2 Sm 0.2 Nd 0.2 )O 1.6863 . In addition, the HEFOs have the best mechanical properties with Vickers hardnesses, flexural strengths and fracture toughnesses of 15.12 GPa, 101.1 MPa and 7.88 MPa-mm 1/2 , respectively, which have potential applications in high-performance structural materials.
研究领域:
材料科学
·
陶瓷工程
✓ 已验证
产品关联
DOI
高影响因子
ChemElectroChem
·
2025
·
IF 3.5
Haoshen Huang,Huafeng Zhou,Nuowen Wu,Haiyang Yu,Weibo Gao,Jianghuan Shi,Jiahao Song,Yayun Zheng,Zhengfei Chen,Zixuan Liu
Graphical A simple carbon black (Ketjenblack, KB)-multiwall carbon nanotubes (MWCNTs) composite was fabricated and used as the air cathode in a Li-O 2 battery, achieving significantly improved specific capacity (up to 10611 mAh/g carbon ), rate capability and cyclability than pristine KB, owing to the synergy of KB's abundant surface area for accommodation of discharge products and MWCNTs’ long-range electronic conductivity. A simple carbon black (Ketjenblack, KB)-multiwall carbon nanotubes (MWCNTs) composite was fabricated and used as the air cathode in a Li-O 2 battery where MWCNTs primarily serve as microscopic cables to enhance long-range electronic conductivity. With optimal KB:MWCNTs mass ratios, the composite exhibited significantly improved specific capacity (up to 10611 mAh/g carbon under 100 mAh/g carbon ), rate capability (up to 9598 mAh/g carbon under 500 mAh/g carbon ) and cyclability than pristine KB, owing to the synergy of KB's abundant surface area for accommodation of discharge products and MWCNTs’ long-range electronic conductivity to guide even and compact deposition of discharge products, and mitigate passivation/clogging of the air cathode surface during discharge. This strategy of using MWCNTs as microscopic cables could also be applied for other commercial materials to construct high-performance and low-cost air cathodes.
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
GREEN CHEMISTRY
·
2011
·Vol. 14
·期 1
·130-135
·
IF 5.472
Bin Li,An-Hua Liu,Liang-Nian He,Zhen-Zhen Yang,Jian Gao,Kai-Hong Chen
Readily available iron compounds were found to be active catalysts for the selective oxidation of sulfide to sulfoxide with molecular oxygen as the oxidant in polyethylene glycol (PEG). As an indispensable component, PEG had a great promotive effect on the reaction. Notably, high conversion (>99%) along with excellent chemo-selectivity of up to 94% could be attained by using Fe(acac)2 as the catalyst at 100 °C. This methodology was proved to be applicable for the transformation of various aromatic and aliphatic sulfides into the corresponding sulfoxides with high selectivity. PEG is considered to play a crucial role in stablizing the Fe(IV)-oxo species formed in situ which is supposed to be responsible for the sulfide oxidation.
研究领域:
有机化学
·
催化化学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）