ACS Applied Energy Materials
·
2022
·
IF 6.959
Sisi Wu,Jing Yang,Ning Qin,Yingzhi Li,Haiou Wang,Yong-Wei Zhang,Qing Wang,Zhouguang Lu
LiO2 is a critical intermediate of oxygen reduction reaction in nonaqueous Li–O2 batteries that largely determines the discharge capacity and cycling stability. Currently, functional redox mediators that can promote the solution reaction route by enhancing the solvation of LiO2 have attracted tremendous interest to increase the attainable capacity. Conversely, redox mediators that quench LiO2 and facilitate the surface reaction route receive little attention. Here, we provide an in-depth exploration of the catalytic pathway and effect of a superoxide quencher that modulates the surface growth of Li2O2. Surprisingly, the predomination of the surface reaction route by ethyl viologen helps deliver a capacity as much as that promoted by the solution reaction route. The findings of this work provide a new direction of screening and evaluating functioning redox mediators for Li–O2 batteries.
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NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 46
·期 30
·14510-14516
·
IF 3.925
Yunxian Zhang,Yongyu Pang,Dong Xia,Guoliang Chai
As a successful alternative to the complex and dangerous anthraquinone process, a simple and safe method for the efficient preparation of hydrogen peroxide is to use the electrochemical two-electron oxygen reduction reaction (2e− ORR) process. Herein, we report a facile approach to achieving metal-free nitrogen-doped carbon material electrocatalysts (N-CMCs) using cheap and easily available raw materials, which also have an excellent electrochemical 2e− ORR catalytic performance and selectivity for hydrogen peroxide (H2O2). The as-fabricated nitrogen-doped carbon material electrocatalysts (named as N-CMC-1 : 5) deliver the high H2O2 selectivity of over 80% in a wide potential range from 0.30 to 0.70 V vs. RHE, where the highest H2O2 selectivity can reach 81.4% at 0.42 V vs. RHE. X-ray photoelectron spectroscopy and electrochemical analyses reveal that the content of pyrrolic-N in the catalysts has a positive effect on the 2e− ORR activity. When the catalyst contains more pyrrolic-N, the catalyst demonstrates a better 2e− ORR performance and H2O2 selectivity in alkaline medium, as well as the long-term stability of the catalyst.
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Nanomaterials
·
2022
·Vol. 12
·期 11
·1931
·
IF 5.719
Shaohong Zang,Xiaorong Cai,Mengshan Chen,Dehong Teng,Fei Jing,Zhe Leng,Yingtang Zhou,Feng Lin
Photocatalytic water splitting is one of the promising approaches to solving environmental problems and energy crises. However, the sluggish 4e−transfer kinetics in water oxidation half-reaction restricts the 2e−reduction efficiency in photocatalytic water splitting. Herein, cobalt vanadate-decorated polymeric carbon nitride (named CoVO/PCN) was constructed to mediate the carrier kinetic process in a photocatalytic water oxidation reaction (WOR). The photocatalysts were well-characterized by various physicochemical techniques such as XRD, FT-IR, TEM, and XPS. Under UV and visible light irradiation, the O2evolution rate of optimized 3wt% CoVO/PCN reached 467 and 200 μmol h−1g−1, which were about 6.5 and 5.9 times higher than that of PCN, respectively. Electrochemical tests and PL results reveal that the recombination of photogenerated carriers on PCN is effectively suppressed and the kinetics of WOR is significantly enhanced after CoVO introduction. This work highlights key features of the tuning carrier kinetics of PCN using charge-conducting materials, which should be the basis for the further development of photocatalytic O2reactions.Keywords:photocatalysis;water oxidation;cobalt vanadates;polymeric carbon nitride
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2022
·Vol. 169
·期 6
·060507
·
IF 4.386
Zining Man,Hao Tian,Xingbao Zhu,Yu Wang,Yuanguo Wu,Xiangyu Wen,Zhe Lü
The solid-state batteries have received widespread attention due to their excellent stability and safety, however, the low ionic conductivity and weak interface contact always restricted its performance. In this work, we propose an in situ thermally cross-linked and solidified polymer electrolyte with polyethylene glycol diacrylate (PEGDA) as scaffold in which succinonitrile (SN) and lithium bis-trifluoromethanesulfonimide (LiTFSI) were further introduced to improve the ionic conductivity. Herein, the composite gel was served as not only solid-solid interface material but also solid-state electrolyte. Different with conventional polymer gels, the solvent evaporation could not happen for this composite material during the solidification process, and therefore resulting in good interface contact without inside bubbles. We further present the investigation on transport principle of Li+ in the solid-state electrolyte and the effect of molecular chain on ionic conductivity. The conductivity of the solid-state electrolyte can reach 1.76 × 10−4 S cm−1 at room temperature without any assistance of liquid electrolytes, which is attributed to the short molecular chain of PEGDA. Electrochemical window of the solid-state electrolyte can reach 5.2 V after cross-linking treatment. And the lithium-oxygen battery using this solid-state electrolyte can stably cycle for more than 1100 cycles with a current density of 200 mA g−1 and a limit capacity of 200 mAh g−1 at room temperature.
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CHEMISTRY-A EUROPEAN JOURNAL
·
2022
·Vol. 28
·期 68
·e202202004
·
IF 5.02
Conghui Zhao,Liwei Sun,Yang Xu,Beibei Dong,Yuhong Luo,Jingde Li,Jianxin Chen,Zisheng Zhang
Graphical Iodine-doped Bi 2 GdO 4 Cl with a significantly promoted visible-light-responsive O 2 -evolving performance of 154.8 μmol ⋅ h −1 and an apparent quantum efficiency of ∼1.1 % at 420 nm is reported. The incorporation of I − ions causes the extended light absorption and promoted charge separation. Visible-light-responsive bismuth-based oxyhalide has recently attracted extensive attention, however, the promotion of its charge separation is still challenging. Herein, we introduce iodine into Bi 2 GdO 4 Cl to synthetize I-doped Bi 2 GdO 4 Cl (denoted as yI−Bi 2 GdO 4 Cl, 0≤y≤2). The incorporation of I − ions is found to enhance light absorption and to accelerate charge separation by combining various characterizations such as density functional theory calculation, photoelectrochemical test, electrochemical impedance spectroscopy, photoluminescence spectrum, and open-circuit voltage decay. The O 2 -evolving performances of 1I−Bi 2 GdO 4 Cl with optimized dopant concentration of I − ion and IrO 2 loaded 1I−Bi 2 GdO 4 Cl are tremendously enhanced by ca. 4 and 45 times compared to pristine Bi 2 GdO 4 Cl. Notably, The O 2 evolution rate reaches as high as 154.8 μmol ⋅ h −1 with an apparent quantum efficiency of ∼1.1 % at 420 nm. The synthetic iodine-doped photocatalyst remains stable after long-term photoreaction, demonstrating its potential in the field of photocatalysis.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Zhaomin Chen,Zhenyu Wu,Jia Xu,Rui Zhao,Xiaoxia Han,Jiwei Jiang,Mingwang Shao,Bin Dong,Zhenhui Kang
Photochemical devices show great potential in applications ranging from electrical energy storage to future smart grids. Here, we report a metal-free composite film cell based on carbon dots (CDots) and polyaniline (PANI), which could achieve 24/7 discharge and photo-charging in seawater. CDots/PANI film cell has an open-circuit-voltage (OCV) of 0.95 V, a maximum power density of 380 mW m 2 , and the ability to discharge continuously for 40 h under solar irradiation of AM 1.5 G. It couples the reduction reaction of PANI, and the CDot-catalyzed oxygen reduction reactions (ORR) during discharge. While the light-induced CDot-catalyzed oxygen evolution reaction (OER) and the reduction reaction of PANI during charging. In particular, in-situ TPV tests were used to verify the effect of the light-induced OER and the kinetic properties of the catalyst on the charge transfer at the interface. We believe this research may provide new ideas for sustainable energy conversion and storage.
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JOURNAL OF NANOBIOTECHNOLOGY
·
2021
·Vol. 19
·期 1
·1-14
·
IF 10.435
Zhang Tian,Zheng Qiang,Fu Yike,Xie Congkun,Fan Gonglin,Wang Yifan,Wu Yongjun,Cai Xiujun,Han Gaorong,Li Xiang
Sonodynamic therapy (SDT), presenting spatial and temporal control of ROS generation triggered by ultrasound field, has attracted considerable attention in tumor treatment. However, its therapeutic efficacy is severely hindered by the intrinsic hypoxia of solid tumor and the lack of smart design in material band structure. Here in study, fine α-Fe 2 O 3 nanoparticles armored with Pt nanocrystals (α-Fe 2 O 3 @Pt) was investigated as an alternative SDT agent with ingenious bandgap and structural design. The Schottky barrier, due to its unique heterostructure, suppresses the recombination of sono-induced electrons and holes, enabling superior ROS generation. More importantly, the composite nanoparticles may effectively trigger a reoxygenation phenomenon to supply sufficient content of oxygen, favoring the ROS induction under the hypoxic condition and its extra role played for ultrasound imaging. In consequence, α-Fe 2 O 3 @Pt appears to enable effective tumor inhibition with imaging guidance, both in vitro and in vivo. This study has therefore demonstrated a highly potential platform for ultrasound-driven tumor theranostic, which may spark a series of further explorations in therapeutic systems with more rational material design. Graphical Abstract
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2021
·
IF 5.816
Shaolong Wang,Dingding Ye,Hao Liu,Xun Zhu,Zhenfei Liu,Rong Chen,Qiang Liao,Yang Yang
The in-situ H 2 O 2 electrosynthesis by two-electron oxygen reduction reaction employing renewable electricity is a promising alternative to traditional anthraquinone process due to its security, environmental friendliness and excellent cost effectiveness, which requires high-performance, cost-effective and environmental-friendly electrocatalysts . A bamboo-derived O-doped rocky electrocatalyst is developed by facile pyrolysis and acid treatment for high-efficiency electroreduction of O 2 to H 2 O 2 . Three-dimensional interconnected hierarchical pores in rocky electrocatalysts expose abundant electroactive sites and facilitate mass transfer of reaction species. From the results of rotating ring-disk electrode test, a H 2 O 2 selectivity up to 80% and superior electrocatalytic activity of the prepared electrocatalyst are achieved by surface oxygen functionalization induced by acid treatment. At the optimal catalyst loading of 2 mg cm −2 , prominent H 2 O 2 productivity of 1037 mmol g c a t a l y s t − 1 h − 1 with high current efficiency up to 74.1% is achieved at 30 mA cm −2 by air-breathing cathode. Higher H 2 O 2 productivity (1525 mmol g c a t a l y s t − 1 h − 1 ) is yielded by further raising the current density to 50 mA cm −2 . Moreover, the durability test of the cathode through ten consecutive runs demonstrates its great stability for electrocatalytic generation of H 2 O 2 . This work inspires the development of promising biomass-derived electrocatalysts for green and sustainable on-site H 2 O 2 electrosynthesis.
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Energy Storage Materials
·
2021
·
IF 17.789
Xiaowei Mu,Chao Xia,Bin Gao,Shuyi Guo,Xueping Zhang,Jianping He,Yonggang Wang,Hao Dong,Ping He,Haoshen Zhou
Rechargeable Li-O 2 batteries have captured increasing attention owing to their ultra-high theoretical specific energy. However, this promising system is confronted with the large overpotential, limited discharge capacity and low cyclic life. Herein, three two-dimensional (2D) molybdenum-based compounds of MoN, MoO 3 and MoS 2 are used as cathode catalysts in Li-O 2 batteries . The catalytic performance and electronic structures of these catalysts are compared comprehensively. Electrochemical test results reveal the superior battery performance of MoN cathodes, which deliver the highest specific discharge capacity of approximately 7400 mAh g − 1 and the lowest discharge/charge overpotential of 0.19/0.72 V. Density functional theory (DFT) calculations demonstrate the metallic property of MoN whereas MoO 3 and MoS 2 are poor conductive. Besides, interface properties between MoN and Li 2 O 2 products as well as reaction pathways of the Li-O 2 battery with MoN cathode are also investigated detailedly by DFT calculations, explaining the excellent catalytic properties of MoN at the atomic level. The present work provides intrinsic insights into designing high-performance cathode catalysts for Li-O 2 batteries with fine-tuned morphology and electronic characteristics.
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TRANSACTIONS OF TIANJIN UNIVERSITY
·
2025
·Vol. 31
·期 3
·278-291
·
IF 8.5
Chi Shuxiu,Wang Chenhui,Liao Jie,Sun Peng,Fei Yaohan,Han You,Zhang Jinli,Wu Jiangjiexing,Li Wei
Aiming at inhibiting the irreversible P2–O2 phase transition of conventional P2-type cathode materials at high voltage and enhancing the cycling stability of sodium-ion batteries, in this article, based on a strategy of adjusting the Na + ion occupancy within the crystal structure, Na 0.67 Ni 0.33 Mn 0.67– x Fe x O 2 (NM– x Fe, x = 0.10, 0.15, 0.20) cathode materials were synthesized by high shear mixer (HSM)-assisted co-precipitation method and evaluated the electrochemical performance at high voltage (4.35 V). The optimal sample NM–0.15Fe exhibits an initial discharge capacity of 130.8 mAh/g (0.1 C), with exceptional retention of 95.9% after 100 cycles (1 C). XRD analysis reveals that Fe intercalation promotes the more amount of Nae-similar occupation; the Nae/Naf ratio equals 1.93 for NM–0.15Fe versus 1.62 for NM, which enhances Na + diffusion kinetics, as confirmed by GITT tests. Through characterizations of in situ XRD, XPS, HRTEM, CV, etc., it is illustrated that the Fe 3+ intercalation can effectively disrupt the Na + /vacancy ordering and inhibit the harmful P2–O2 phase transition, and then improve the cycling stability of the cathode. DFT calculations disclose that intercalated Fe can reduce the electron densities of adjacent transition metallic elements, generating more repulsive forces impacted on sodium and consequently appearance of more Nae sites, leading to a lower Na + diffusion energy barrier. Such strategy of modulating Na occupation sites in crystal structure is conducive to the development of low-cost and high-performance layered cathode materials for sodium-ion batteries.
研究领域:
电化学储能
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材料科学
·
固态化学
·
能源材料
·
电池技术
·
过渡金属氧化物
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Communications Chemistry
·
2025
·Vol. 8
·期 1
·389
·
IF 6.2
Han Lei,Tan Jingying,Zhang Yucui
Given the promising prospect of nanozymes in colorimetric test strips, it is essential to eliminate the interferences of their multi-activities and various colors on the test strip. Here, white Mn-based metal-organic frameworks (Mn-MOFs) with ultrathin 2D morphology (3 nm thick) were successfully synthesized by a simple ultrasonic approach. The origin of the white optical property in Mn-MOFs was systematically investigated, revealing that it stems from specific metal-ligand coordination polymerization rather than morphological features or defect states. Mn-MOF nanozymes possessed exclusive peroxidase-mimicking activity rather than oxidase-like activity, effectively resisting O 2 interference during colorimetric assay. Moreover, Mn-MOF nanozymes displayed unique substrate selectivity without additional modification. Unlike other colored nanozymes, the whiteness of Mn-MOF nanozymes enhanced the paper’s whiteness, boosting contrast for colorimetric detection on test strip. This study pioneers a systematic investigation into the origin of whiteness in MOF nanozymes. The coordination-defined properties enable interference-free optical design and O 2 -resistant on-site detection.
研究领域:
材料科学
·
纳米技术
·
分析化学
·
生物传感器
·
酶模拟
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JOURNAL OF MATERIALS SCIENCE
·
2025
·Vol. 60
·期 48
·25148-25163
·
IF 3.9
Zhang Zhenyan,Chai Huan,Yu Zhengqian,Li Jinsheng,Li Pengfei,Wu Lei,Li Zhanshuai,Qi Xiwei
TiO 2 -based materials are widely used in high-temperature capacitors and aerospace electronics but face challenges such as high dielectric loss and limited thermal stability in conventional single-component systems. To address these issues, we propose a novel strategy integrating high-entropy doping design and oxygen vacancy engineering. In 2 O 3 -doped (GeMnTiSnMo)O 2 high-entropy ceramics (GMTSMO- x In, x = 0.1–1) were synthesized via solid-state reaction. Experimental results reveal that In 3+ doping generates high-density oxygen vacancies (V o ·· ) through charge compensation, forming [Ti 3+ - V o ·· -Ti 3+ ] and [Mn 3+ - V o ·· -Mn 3+ ] defect-dipole clusters. These clusters enhance electron localization and suppress carrier migration, reducing dielectric loss by threefold. Simultaneously, oxygen vacancy enrichment strengthens interfacial polarization, increasing the dielectric constant by fourfold. The optimal GMTSMO-0.5In exhibits a relative permittivity ( ε r ) of 4.0 × 10 6 and a low loss tangent of 15 at 650 ℃/100 Hz, outperforming traditional TiO 2 -based materials and existing high-entropy oxides. All compositions demonstrate excellent temperature stability (25–400 ℃) and frequency-independent behavior above 10 4 Hz. This work provides a high-entropy-driven approach for dynamic defect engineering, paving the way for advanced dielectric materials in extreme-condition energy storage systems.
研究领域:
材料科学
·
陶瓷与介电材料
·
电子材料
·
储能技术
·
缺陷化学
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