APPLIED CATALYSIS B-ENVIRONMENTAL
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2018
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IF 11.698
Anye Shi,Huihui Li,Shu Yin,Zaili Hou,Jiayue Rong,Jiachi Zhang,Yuhua Wang
Cs x WO 3 nanorods can be used to sensitize the single layer g-C 3 N 4 , where full spectrum light harvesting excited electrons to drive the photocatalytic reduction of N 2 into NH 3 . Under UV light, both water splitting and solar ammonia synthesis reaction exhibit high activity. However, selectivity towards ammonia over hydrogen is realized under NIR irradiation. With the control of methanol, O 2 can directly decide the NH 3 or H 2 evolution on photocatalyst. The origin is the strong capture of O 2 with the electrons from the photocatalyst under light irradiation to yield the oxygen active species, which transfer electrons subsequently with help of methanol to generate NH 3 . However, H 2 production will be suppressed by O 2 . And with its sacrifice, methanol preserves the produced NH 3 from oxidation. The O 2 -sacrificial agent mediated NH 3 evolution reaction found here provides insights in the promotion role of them in other catalysis.
研究领域:
材料科学
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环境科学
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化学工程
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DOI
高影响因子
ACS Applied Energy Materials
·
2021
·
IF 6.024
Shidong Song,Dequan Zhang,Yanli Ruan,Limei Yu,Yongqiang Xu,Joykumar Thokchom,Donghai Mei
Heightened attention for solid-state Li–O2 batteries (SSLOBs) exists due to their improved safety, wider electrochemical window, and high energy density in addition to the solid electrolyte’s innate capability of suppressing Li dendrite penetration and shielding the Li metal anode from oxygen, CO2, and moisture in the air, in comparison with the conventional Li–O2 batteries using liquid organic electrolytes. Herein, a cathode supported quasi-SSLOB with an integrated composite polymer-based architecture (ICPA) is developed with reduced interfacial resistance, extended triple-phase boundaries (TPBs) for Li–O2 reactions, and a thin film solid-state electrolyte. The Li–O2 cell with ICPA (denoted as ICPA cell) exhibits a lower charge transfer impedance than its counterpart with the same composite polymer electrolyte (CPE) but a nonintegrated structure (termed the CPE cell). The former shows reduced interfacial impedance between electrolyte and cathode and increased TPBs. Furthermore, the ICPA cell delivers higher discharge capacity, lesser capacity decay, and significantly lower impedance rise after cycles than the CPE cell, ascribed to the continuous Li-ion transport in ICPA and the resulting more efficient discharge and charge processes. Under a limited capacity cycling protocol of 300 mAh g–1, the ICPA cell achieves excellent reversibility for 78 cycles, remarkably surpassing the CPE cell which only performs 44 cycles in addition to showing half of the after-cycle impedance compared to that for the CPE cell. Nonetheless, the same composite polymer electrolyte used for both CPE- and ICPA-based cells demonstrates excellent stability toward Li metal after long-term cycling. These findings manifest that the design and application of cathode supported SSLOB with ICPA can be a promising approach to achieve high-performance Li–O2 batteries.
研究领域:
材料科学
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电化学
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能源存储技术
✓ 已验证
DOI
高影响因子
CERAMICS INTERNATIONAL
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2024
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IF 5.1
Xinyu Ping,Bin Meng,Xiaohua Yu,Qingqing Yang,Zhiyuan Ma,Xiaoyu Pan
A medium-entropy fluorite-structured ceramic of (Y 0·25 Zr 0.25 Hf 0.25 Ce 0.25 )O 2−δ was prepared using a solid state reaction method combined with conventional sintering at 1600 ° C for 10 h. This ceramic has uniform elemental distribution without impurity and segregation. The annealing experiment results show a reversible transformation between single phase and double phases in (Y 0·25 Zr 0.25 Hf 0.25 Ce 0.25 )O 2−δ in 800–1600 °C. The reversible phase transformation does not display any obvious influence on the thermal expansion of this sample. The thermal expansion coefficient of (Y 0·25 Zr 0.25 Hf 0.25 Ce 0.25 )O 2−δ is 12.4 × 10 −6 K −1 in 100–1500 °C, higher than that of 8 wt% yttria-stabilized zirconia (8 YSZ). Furthermore, (Y 0·25 Zr 0.25 Hf 0.25 Ce 0.25 )O 2−δ possesses a lower thermal conductivity (1.51 W m −1 K −1 at 900 ° C) and higher oxygen barrier property compared with 8 YSZ at high temperature. The Vickers' hardness, Young's modulus and fracture toughness of (Y 0·25 Zr 0.25 Hf 0.25 Ce 0.25 )O 2−δ are 10.0 GPa, 193.9 GPa and 1.93 MPa m 1/2 , respectively. These results demonstrate that (Y 0·25 Zr 0.25 Hf 0.25 Ce 0.25 )O 2−δ can be used as a promising candidate ceramic of thermal barrier coatings.
研究领域:
材料科学
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热物理性质
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陶瓷材料
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产品关联
DOI
高影响因子
Materials Today Communications
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2024
·
IF 3.7
Zhiqin Wen,Zhenyu Wu,Bo Ma,Jiedong Qin,Li Tang,Taoyi Lu,Yuhong Zhao
A novel 6-cationic single-phase high-entropy fluorite oxides (HEFOs) (Ce 0.16 Zr 0.16 La 0.16 Sm 0.16 Nd 0.16 Y 0.16 )O 2- δ (CZLSNYO) have been prepared by using solid-state reactions, and the structure and mechanical properties of the HEFOs were studied in depth. CZLSNYO exhibits a single-phase cubic fluorite structure with a smooth and crack-free surface and distinct grain boundaries after sintering at 1400 °C, 1500 °C and 1600 °C for 12 hours. The concentration of Ce 3+ in Ce ions is calculated to be 22.23 % ± 1.11 %, and the value of δ is 0.3519 ± 0.0176, yielding a nominal composition of (Ce 0.16 Zr 0.16 La 0.16 Sm 0.16 Nd 0.16 Y 0.16 )O 1.6481 ± 0.0176 . With the increase of sintering temperature, the average grain size of CZLSNYO initially enlarges and then reduces, and its Vickers hardness exhibits a comparable trend. By comparing with the 5-cations (Ce 0.2 Zr 0.2 La 0.2 Sm 0.2 Nd 0.2 )O 2- δ HEFOs, 6-cationic single-phase CZLSNYO sintered at 1500 °C possess large hardness (16.32 GPa) and fracture toughness (8.07 MPa m 1/2 ), since the addition of Y element increases the configuration entropy of the system, and Y has a greater hardness, resulting in a cocktail effect.
研究领域:
材料科学
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化学
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产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Haonan Zhang,Changhe Lu,Shuai Wang,Qinhua Zhang,Qiang Zhou,Shuxu Zhu,Chong Qi,Mingbo Wu,Wenting Wu
The utilization of O 2 for propylene epoxidation is a highly desirable reaction due to its 100 % atom economy. However, achieving this reaction under mild conditions presents a significant challenge. In this paper, we present a tandem reaction system that combines 4,4′-dibromobenzophenone (BP) modified carbon nitride (g-C 3 N 4 ) with titanium silicalite zeolite (TS-1) to enable the selective photooxidation of propylene into propylene oxide at room temperature, using O 2 as the oxygen source. The achieved production rate of propylene oxide was an impressive 1195 μmol/g cat. /h, with a selectivity exceeding 99 %. Furthermore, the catalyst exhibited no significant deactivation after 5 cycles. Spectra and in-situ capture experiments revealed that the reaction involved a two-step system, with photocatalytic production of H 2 O 2 and propylene epoxidation facilitated by H 2 O 2 ·H 2 O 2 was generated through O 2− and 1 O 2 pathways, with an in-situ utilization efficiency of H 2 O 2 reaching 82 %. This work presents a novel approach for the direct epoxidation of propylene using O 2 .
研究领域:
化学工程
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环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
LANGMUIR
·
2025
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IF 3.9
Dexi Yu,Yuhong Lin,Wenhui Zhou,Xiaoyi Wang,Zhenzhen Yu,Yidong Hou,Masakazu Anpo,Jimmy C. Yu,Jinshui Zhang,Xinchen Wang
Photocatalytic oxidation of benzene to phenol using molecular O2 is one of the most promising sustainable approaches for the green synthesis of phenol. Introducing oxygen vacancies (OVs) on semiconductor surfaces by defect engineering is a promising strategy to enhance the efficiency of benzene oxidation to produce phenol due to the unique functions of OVs in facilitating the charge separation and activation of molecular O2. Herein, a vacuum-sealed annealing strategy has been well developed to generate abundant surface OVs on semiconductors, such as WO3. The well-sealed quartz vial creates a well-controlled low-pressure condition for the formation of OVs without the need for external energy for maintaining the vacuum state. Moreover, the gaseous species generated during the thermal annealing process help mitigate stress-induced defects, particularly bulk defects. The vacuum-sealed annealed WO3 with sufficient OVs and reduced bulk defects shows a better photocatalytic performance in the one-step oxidation of benzene to phenol with O2, compared to the WO3 synthesized through thermal annealing in Ar and H2 atmospheres. The present vacuum-sealed annealing strategy is found to be further applicable to engineer a wide range of semiconducting photocatalysts with abundant OVs to optimize their properties for efficient photocatalysis and other OV-promoted systems.
研究领域:
材料科学
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环境科学
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化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
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IF 9.7
Jianying Xi,Yong Li,Longhao Lv,Zhengshuai Tang,Fangfang Liu,Jinliang Liu
Photodynamic (PDT) and chemodynamic therapies (CDT) relying on reactive oxygen species-mediated treatments mainly face various challenges of hypoxia, endogenous hydrogen peroxide (H 2 O 2 ) deficiency, and glutathione (GSH) overexpression in the tumor microenvironment. Herein, we propose a novel strategy using a core–shell structured nanocomposite, UCNP@mSiO 2 @5-ALA-CaO 2 -Cu(UA@CC). The strategy centers on upconverting NPs and then utilizes mesoporous silica loaded with 5-aminolevulinic acid (5-ALA) to maximize the enrichment of protoporphyrin IX (Pph IX), an intra-tumor photosensitizer. Then in the acidic tumor microenvironment (TME), CaO 2 in the outer layer reacts with H 2 O to form O 2 , H 2 O 2 and Ca 2+ , and the released H 2 O 2 serves as an auxiliary “fuel” to induce acceleration of the Fenton-like (Cu 2+ ) reaction and inactivation of the antioxidant GSH enzyme, thus enhancing the tumor cells’ Catalysis. Furthermore, under the excitation of a 980 nm laser, 5-ALA-mediated PDT and Cu + -based CDT were initiated. Through interconnected processes of Ca 2+ overload, self-supply of H 2 O 2 /O 2 , and enhanced GSH depletion, an accelerated cycling strategy for combined PDT/CDT therapy was established, resulting in amplified oxidative stress and anti-tumor capabilities, which was validated in cancer cells and melanoma mouse models.
研究领域:
肿瘤学
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纳米医学
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生物化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING SCIENCE
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2026
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IF 5.1
Akkammagari Putta Rangappa,Wei Xiong,Xinxin Lu,Guohan Sun,Yixuan Liu,Jiangdong Dai,Jun Zhao
CTAB assisted synthesis of FeS 2 allows precise control over surface sulfur vacancies. • Surface-modified FeS 2 boosts O 2 activation and enhances reactive oxygen species (ROS) population. • Vs-rich FeS 2 lowers HMF conversion barrier, giving 15.73 fold higher DFF yield than pristine FeS 2 . • Synergy of Vs and Fe redox cycling in FeS 2 accelerates charge transfer and surface reactivity. • Tuning defects and redox states in FeS 2 enable sustainable and versatile photocatalysis. The photocatalytic conversion of 5-hydroxymethylfurfural (HMF) to 2,5-diformylfuran (DFF) using molecular oxygen (O 2 ) as the oxidant offers a sustainable route for biomass valorization, yet is limited by inefficient O 2 adsorption and activation on conventional photocatalysts. Herein, we report a Cetrimonium bromide (CTAB) assisted synthesis of iron pyrite (FeS 2 ) with engineered surface sulfur vacancies (Vs) that enable simultaneous activation of O 2 and HMF under solar light. Introduction of Vs increases the catalyst’s specific surface area and modulates the local electronic structure, particularly tuning the Fe 2+ /Fe 3+ redox landscape. These defect sites act synergistically, where Fe 2+ sites act as preferred O 2 adsorption centers, while adjacent Vs promote electron localization and transfer to adsorbed O 2 , thereby facilitating its activation through the oxidation of Fe 2+ to Fe 3+ . Concurrently, the modulated Fe redox states enable efficient HMF adsorption and oxidation through interaction with the activated O 2 species (•O 2 – and 1 O 2 ). This dual activation mechanism, driven by vacancy engineering and Fe redox dynamics, enhances charge transfer kinetics and surface reactivity, leading to a 15.7-fold increase in DFF production compared to prismatic FeS 2 . Our findings emphasize the critical role of Vs and Fe 2+ /Fe 3+ redox interplay in organizing simultaneous O 2 activation and HMF oxidation, advancing the rational design of efficient photocatalysts for biomass-derived chemical production. Download: Download high-res image (117KB) Download: Download full-size image
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DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2026
·Vol. 14
·期 35
·16045-16056
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IF 7.6
Ge Xiao,Wu Xinyi,Liu Xinya,Zheng Xiyang,Xu Jinze,Tian Li-jiao,Wang Wei,Wang Xiaozhi
Spin state strongly governs the pathway selectivity of photocatalytic oxygen reduction, dictating whether the reaction proceeds via the desired two electron (2e – ) route to H 2 O 2 or the competing four electron (4e – ) pathway. Herein, this work reports a ligand-field symmetry-breaking strategy that enables controlled spin state switching, thereby steering the oxygen reduction pathway toward selective two electron H 2 O 2 production. Specifically, symmetry breaking creates an asymmetric equatorial ligand field, triggering a deterministic spin state transition from intermediate spin to high spin on the Mn site. The resulting high-spin configuration features delocalized d-states and a downshifted d-band center, which collectively weaken *OOH adsorption to suppress premature O–O bond cleavage while preserving efficient O 2 activation through spin polarized electron transfer. As a result, the optimized high spin catalyst delivers an exceptional H 2 O 2 production rate of 5025 μmol·g –1 ·h –1 under simulated sunlight, representing a 2.3-fold enhancement over its intermediate spin (IS) counterpart. Furthermore, its activity is maintained under natural sunlight in ambient air, achieving a H 2 O 2 production rate of 2662 μmol·g –1 ·h –1 . This work establishes ligand field symmetry breaking as a precise and generalizable paradigm for spin state engineering in single atom catalysis, offering a direct route to overcome the selectivity efficiency compromise in photosynthesis of H 2 O 2 .
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产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2025
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IF 8.2
Yingdong Hao,Yonghui Zhao,Jun Ma,Xinru Han,Yingxiao Wang,Pengyu Chen,Deng Hu,Yuefeng Liu,Wei Wei,Nannan Sun
Photocatalytic oxidation of methane (CH4) to high value-added liquid oxygenates with oxygen (O2) as an oxidant has long been a promising process. In addition to the activation of CH4, the selective reduction of O2 to hydroperoxyl (·OOH) is also a crucial factor in determining the efficiency and selectivity of the overall reaction. In thermal catalysis, strong interactions between oxygen vacancies (OVs) on the catalyst surface and O2 are widely adopted as a means of enhancing O2 activation. However, reports of this phenomenon are limited in photocatalysis; this is attributable to the fact that the reduction of O2 is dependent upon its reaction with photogenerated electrons (e–). For the majority of photocatalysts, the transfer of e– to metal cocatalysts results in the spatial separation of e– from OVs. Therefore, the intrinsic affinity between OVs and O2 is not fully exploited. In this study, we discovered that H2 treatment at elevated temperatures on ZIF-8-derived ZnO led to the formation of an OV-enriched amorphous layer on the surface. After the introduction of the Ag cocatalyst, the as-prepared Agx-OVs/ZnO exhibited an unconventional carrier transfer direction, whereby photogenerated e– and holes (h+) are transferred to OVs and Ag, respectively. As a result, the preferential O2 adsorption and activation sites can be spatially combined together on the OVs and thus drive the reduction of O2 to realize efficient and directed generation of ·OOH. In parallel, the transfer of h+ to the Ag sites weakens its oxidation capability and avoids overoxidation while ensuring CH4 activation. The optimized defect-rich Ag0.5-OVs/ZnO-z photocatalyst reaches a high liquid oxygenate yield of 10148 μmol gcat–1 h–1 with 95% selectivity and a high TOF of 2.4 × 106 μmol gAg–1 h–1. This work sheds new light on the design of photocatalytic CH4 oxidation catalysts via manipulation of carrier transfer direction.
研究领域:
化学
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材料科学
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环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
BIOMATERIALS
·
2018
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IF 8.806
Shutao Gao,Pengli Zheng,Zhenhua Li,Xiaochen Feng,Weixiao Yan,Shizhu Chen,Weisheng Guo,Dandan Liu,Xinjian Yang,Shuxiang Wang,Xing-Jie Liang,Jinchao Zhang
Improving the supply of O 2 and the circulation lifetime of photosensitizers for photodynamic therapy (PDT) in vivo would be a promising approach to eliminate hypoxic tumors. Herein, by taking advantage of the significant gas-adsorption capability of metal-organic frameworks (MOFs), a biomimetic O 2 -evolving photodynamic therapy (PDT) nanoplatform with long circulating properties was fabricated. Zirconium (IV)-based MOF (UiO-66) was used as a vehicle for O 2 storing, then conjugated with indocyanine green (ICG) by coordination reaction, and further coated with red blood cell (RBC) membranes. Upon 808 nm laser irradiation , the initial singlet oxygen ( 1 O 2 ) generated by ICG would decompose RBC membranes. At the same time, The photothermal property of ICG could facilitate the burst release of O 2 from UiO-66. Subsequently, the generated O 2 could significantly improve the PDT effects on hypoxic tumor. Owing to the advantages of long circulation and O 2 self-sufficient, the designed nanotherapeutic agent can improve the efficiency of treatment against hypoxia tumor via PDT. Hence, this study presents a new paradigm for co-delivery of O 2 and photosensitizers, and provides a new avenue to eliminate hypoxic tumors.
研究领域:
生物医学工程
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纳米技术
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癌症治疗
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材料科学
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产品关联
DOI
PubMed
高影响因子
MOLECULES
·
2024
·Vol. 29
·期 23
·5622
·
IF 4.2
Shengxue Zhang,Wangchuan Xiao,Jingjing Wu,Fanhong Wu,Houjin Huang,Xiaoyu Ma,Yafei Shi,Chao Liu
A novel and efficient 1,2-oxidative trifluoromethylation of olefins employing Ag(O 2 CCF 2 SO 2 F) as a trifluoromethyl source is described with O 2 as the oxidant, which provides access to a variety of valuable α-trifluoromethyl-substituted ketones. The broad substrate scope, feasibility of large-scale operation, and derivatization reactions of α-trifluoromethyl ketones demonstrate the promising utility of this protocol.
研究领域:
有机化学
·
合成化学
✓ 已验证
DOI
PubMed
高影响因子
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