ACTA PHYSICO-CHIMICA SINICA
·
2025
·
IF 13.5
Yanyan Zhao,Zhen Wu,Yong Zhang,Bicheng Zhu,Jianjun Zhang
Photocatalytic oxygen reduction reaction (ORR) offers a mild and cost-effective approach for hydrogen peroxide (H 2 O 2 ) production. However, its practical application is significantly hindered by rapid charge carrier recombination and insufficient O 2 adsorption capacity in photocatalysts. To address these limitations, we developed a strategy involving the creation of S-vacancy-rich CdIn 2 S 4 (S v –CIS) to facilitate charge separation and subsequent deposition of Au nanoparticles on its surface (Au–S v –CIS) to strengthen O 2 adsorption. The results suggest that the optimized Au–S v –CIS achieves a significantly increased H 2 O 2 production yield of 2542 μmol·h·g −1 in 10%-ethanol/water solution, which is about 12.8 and 1.7 times higher than that of pure CIS and S v –CIS. Comprehensive characterizations including photoluminescence spectra, time-resolved photoluminescence spectra, transient photocurrent response, electrochemical impedance spectra, and femtosecond transient absorption spectroscopy confirm the improved charge dynamics of Au–S v –CIS. In addition, temperature-programmed desorption of O 2 combined with density functional theory calculations conclusively demonstrates the superior O 2 adsorption capacity of Au–S v –CIS. This work provides a design strategy for efficient solar–to–chemical energy conversion through cooperative photocatalyst engineering.
研究领域:
光催化
·
纳米材料
·
能量转换
·
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
Energy & Environmental Materials
·
2025
·
IF 14.1
Zhengcai Zhang,Dulin Huang,Xiaohui Peng,Zhang Zhang,Yaying Dou,Zhen Zhou
Redox mediators (RMs) represent the most promising strategy to address the sluggish kinetics of lithium–oxygen (Li–O 2 ) batteries. To achieve high-energy and cost-effective Li–O 2 batteries, carbon materials are typically regarded as ideal cathodes in these systems. However, the impact of their surface properties—which often regulate specific discharge pathways—on the RM-mediated oxygen reduction reaction (ORR) remains unclear. In this study, CNTs electrodes with different surface properties are fabricated. Results suggest that CNTs with more surface defects not only promote the unmediated discharge pathway even in RMs-involved battery systems but also exacerbate the corrosion of carbon cathodes. This, in turn, leads to the undesired accumulation of Li 2 O 2 and Li 2 CO 3 on the cathode surface, which hinders effective and continuous electron transfer between the cathode and RMs, ultimately decreasing the catalytic activity of RMs. As a result, the discharge capacity of the battery is seriously diminished, especially at large current densities. These findings underscore the significance of surface engineering in advancing the performance of RMs-assisted Li–O 2 batteries.
研究领域:
电化学
·
材料科学
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储能技术
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表面工程
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电池技术
✓ 已验证
产品关联
DOI
高影响因子
Nano Materials Science
·
2025
·
IF 17.9
Hongjing Liu,Shan Ren,Xiaodi Li,Liang Wang,Bofeng Bai,Shouning Chai,Peng Chen,Fan Dong
Photocatalytic oxidation of nitrogen oxides (NO x ) is a promising technology for environmental protection and green sustainable development. However, its practical application remains limited due to inefficient activation of NO and O 2 , stemming from inadequate structural design of photocatalysts. Herein, we developed a thin-layer two-dimensional (2D) material Bi 2 MoO 6 (BMO) via cetyl trimethyl ammonium chloride (CTAC) addition in synthesis process, which effectively modulates the surface electronic structure, enhance the light absorption and activation of NO and O 2 . This thin-layer Bi 2 MoO 6 nanosheets achieved a NO oxidation efficiency of 45.3 %, which was about 5.5 times that of traditional bulk BMO (8.2 %). Additionally, it demonstrated superior selectivity for NO 2 − /NO 3 − production (86.6 %) compared to bulk BMO (60.5 %) and significantly reduced the formation of toxic NO 2 byproducts (13.4 % vs. 39.5 %). Combining experimental characterizations and density functional theory (DFT) simulations, it demonstrated that the electron-hole pair separation could be promoted and targeted adsorption activation of O 2 can be enhanced to form superoxide radicals (•O 2 − ) and singlet oxygen ( 1 O 2 ) via the effect of surface charge transfer adjustment on the thin-layer structure of Bi 2 MoO 6 , which are key factors affecting the efficiency and selectivity of photocatalytic oxidation of NO. This work provides important insights into the formation of directed ROS and proposes a unique mechanism for selective NO oxidation.
研究领域:
环境科学
·
材料科学
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光催化
·
化学工程
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理论化学
✓ 已验证
产品关联
DOI
高影响因子
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
✓ 已验证
DOI
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2025
·
IF 11.3
Jingwen Qian,Mingyi Yu,Zheng Lian,Shule Zhang,Qin Zhong
An innovative strategy in wet flue gas denitration technology was proposed to control nitrogen oxide emissions from cement kiln. Here the use of tetrabutylammonium bromide (TBAB) as an additive improved the absorption and utilization efficiency of sulfite absorbents for NO2. Compared with the sulfite solution, the stability time and absorption efficiency of adding TBAB were increased from 25 to 76 min and from 91.2 to 98.4%, respectively. Continuous absorption for 480 min indicated the feasibility of TBAB for repeated use. Moreover, we propose an antioxidant mechanism, including the capture of SO3•– by TBA+, and the reduction of SO3•– by Br–. The successive steps kept the sulfite from the cyclic depletion of the radical chain reaction of “Generate SO3•–-Introducing O2–Consuming SO32–” due to O2. A new application of TBAB in free radical trapping and antioxidant is given. Furthermore, a kinetic model describing the macroscopic absorption rate was developed based on different operating conditions.
研究领域:
环境化学
·
化学工程
·
物理化学
·
大气污染控制
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工业生态学
✓ 已验证
产品关联
DOI
PubMed
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
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材料科学
·
化学动力学
·
可再生能源
·
环境化学
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Yingnan Zhu,Jiahang Si,Tiantian Xu,Lan Zheng,Xinyu Xiao,Xiaohan Sun,He Ding,Yuze Dong
Chemodynamic therapy (CDT) and photodynamic therapy (PDT) have emerged as promising strategies for treating skin abscesses. However, their therapeutic efficacy is fundamentally constrained by the hypoxic and hydrogen peroxide-deficient microenvironment characteristic of abscesses. Herein, we developed a near-infrared (NIR) light-responsive nanoplatform (ICG/CuO2@PCM) by encapsulating copper peroxide (CuO2) and indocyanine green (ICG) within a phase-change material (PCM), which enables control over self-supplied H2O2/O2 release via an NIR-triggered cascade. Upon irradiation, ICG-mediated photothermal conversion elevates the temperature beyond the PCM melting threshold, triggering a burst release of CuO2 and ICG. CuO2 generates hydroxyl radicals (•OH) through a Fenton-like reaction in the acidic wound microenvironment. Additionally, CuO2 can thermally decompose under photothermal conditions to produce a sustained oxygen supply, which ICG immediately converts into singlet oxygen (1O2), thereby enhancing PDT efficiency. Furthermore, photothermal therapy not only enhances the efficiency of CDT but also provides additional antibacterial support. Remarkably, ICG/CuO2@PCM (NPs), coupled with irradiation, accelerate abscess wound recovery by dispersing biofilm, killing bacteria, and promoting macrophage polarization toward an anti-inflammatory phenotype. Overall, this NIR-responsive nanoplatform highlights the promise in controlled modulation of microenvironment-adaptive antimicrobial strategies to overcome current limitations of hypoxic infections.
研究领域:
生物医学工程
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纳米医学
·
感染性疾病治疗
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抗菌治疗
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转化医学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Cailiang Yue,Yukun Tian,Linlin Zhu,Nan Sun,Zhiqi Zhou,Fuqiang Liu,Yifei Sun
Photocatalytic 1 O 2 generation has emerged as a promising technology for environmental remediation and organics synthesis. Nevertheless, the efficiency of photocatalytic 1 O 2 generation via O 2 activation through charge-transfer mechanism remains challenging in carbon nitride due to the weak dielectric screening effect. Herein, series of uric acid (UA)-modified ultrathin carbon nitride nanosheets (UCN-x) were fabricated by the simple supramolecular self-assembly process. Comprehensive characterizations revealed that the incorporation of UA pigment would induce purine structure into heptazine skeleton. Photocatalytic experiments showed that the modification of UA greatly enhanced photocatalytic 1 O 2 generation ability. The optimal UCN-2 exhibited superior photocatalytic degradation of tetracycline (TC) with the normalized TC degradation rate up to 10.03 mg TC g cat −1 min −1 , which was 2.1–31.1 times as high as that of reported photocatalysts. What's more, UCN-2 exhibited excellent photocatalytic TC degradation across diverse aqueous conditions, demonstrating significant potential in environmental remediation. Time-dependent density functional theory (TD-DFT) calculation revealed that the doping of UA could trigger the spatial separation of h + /e − distribution, with h + concentrated in UA pigment and e − concentrated in adjacent heptazine ring. The engineered adjacent redox sites were precisely tailored to align with the charge-transfer mechanism for photocatalytic 1 O 2 generation. This work established a fundamental framework for designing highly efficient photocatalysts with manipulated O 2 activation.
研究领域:
环境科学
·
材料化学
·
光催化
·
纳米材料
·
环境修复
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Yixi Wang,Wenqing Xu,Zhi Liu,Yulong Shan,Wanrong Chen,Xinyu Zhang,Tingyu Zhu
Controlling both CO and NOx pollutants without additional cost is necessary but challenging, especially in industrial flue gas with complex components. Previous studies mainly focused on the effect of O 2 and SO 2 on the CO oxidation side reaction and valence state of Ir species on various catalysts, while neglecting the impact on NO conversion pathway. Herein, we propose an "ineffective reaction pathway" in the presence of O 2 with nitrate as an intermediate according to the results of in situ DRIFTS and DFT. And we also reveal the contribution of SO 2 in inhibiting the adsorption of O 2 and promoting the selective adsorption of NO and CO even at lower injection concentrations, based on the oxidation of SO 2 on Ir(111). This is quite a favorable characteristic for the treatment of industrial flue gas, resolving the long–standing dispute on the involvement of these components in the CO–SCR reaction. Under specific conditions (CO/NO=20, O 2 =5%, SO 2 =200 ppm) at 250 °C, the NOx conversion is as high as 78%. These results will contribute to the development of more efficient catalysts in the future for simultaneously controlling two pollutants (CO and NOx).
研究领域:
环境科学
·
催化化学
✓ 已验证
产品关联
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
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Energy Materials
·
2025
·Vol. 5
·期 11
·N
·
IF 11.2
Shukai Liu,Huang Tan,Gaole Dai,Shiyun Xiong,Yu Zhao,Benxia Li
The oxygen evolution reaction (OER), as a pivotal process in electrochemical water splitting, directly determines energy conversion efficiency. Ruthenium (Ru)-based catalysts have gained considerable attention in recent years due to their decent intrinsic activity in acidic media. Previous studies have demonstrated that while Ru exhibits superior OER activity compared to RuO2 in acidic environments, its operational stability remains markedly inferior. This performance dichotomy, coupled with the persistent challenges of active species dissolution and catalyst particle aggregation during prolonged operation, significantly hinders their practical implementation in electrochemical systems. To address these challenges, this study develops a carbon nanotube (CNT)/Fe-Ni@RuO2@PANI-350 composite catalyst composed of RuO2 nanoparticles supported on bimetallic Fe-Ni modified CNTs (CNT/Fe-Ni) and encapsulated with polyaniline (PANI). This catalyst utilizes the anchoring effect of bimetallic Fe-Ni sites and the spatial confinement effect of PANI coating layer, effectively inhibiting the dissolution and agglomeration of RuO2 during both high-temperature processing and electrochemical operation, thereby significantly enhancing electrochemical stability. The anchoring strength of RuO2 nanoparticles on CNT/Fe-Ni support via the nano-confinement effect, as well as the microscopic mechanisms underlying the performance enhancement, are revealed by density functional theory calculations and experimental characterizations. The composite catalyst demonstrates fascinating OER performance in 0.5 M H2SO4, exhibiting a low Tafel slope of 39.1 mV dec-1 as well as low overpotentials of 188 and 225 mV at current densities of 10 and 100 mA cm-2, respectively. Remarkably, the composite catalyst demonstrates significantly enhanced stability, exhibiting only ~30 mV overpotential increase during 150 h continuous operation at 10 mA cm-2. This study highlights a simple yet effective nano-confinement strategy to address the challenges of Ru-based catalysts, and provides a practical paradigm for designing and preparing highly efficient OER electrocatalysts with enhanced stability.
研究领域:
电化学
·
催化
·
纳米材料
·
能量转换
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Yu Luo,Chenchen Liu,Jiahui Liu,Xueming Liu,Yang Zhou,Xinwen Ou,Bo Weng,Jin Jiang,Bin Han
Photocatalytic O 2 reduction presents a sustainable strategy for H 2 O 2 synthesis, while the in-situ decomposition of H 2 O 2 significantly deteriorates the activity and stability. Here, by introducing anthraquinone centers into covalent organic frameworks (DQTb-COFs), for the first time, we realized the suppression of in-site decomposition of generated H 2 O 2 via site-engineering of COFs. Under visible light irradiation, DQTb-COFs achieves an H 2 O 2 generation rate of 1844.1 μmol h −1 g −1 without sacrificial agents, which is about 3.4 times that of its counterpart without anthraquinone centers (DATb-COFs). The generated H 2 O 2 on DATb-COFs is readily reduced into hydroxyl radicals (•OH), which is not observable on DQTb-COFs. Experiments and calculations demonstrated that the anthraquinone centers of DQTb-COFs can enhance the generation of H 2 O 2 by facilitating the utilization of O 2 and promoting the desorption of H 2 O 2 . This work highlights how to inhibit the in-situ decomposition of H 2 O 2 via site-engineering of COFs, and blazes a new trail for highly efficient H 2 O 2 photosynthesis.
研究领域:
材料科学
·
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）