NEW JOURNAL OF CHEMISTRY
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2022
·Vol. 46
·期 18
·8739-8751
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IF 3.925
Quansheng Wu,Songhua Zhou,Chengbing Fu,Jiesong Zhang,Bo Chen,Hongyan Pan,Qian Lin
For the mono-metal Pd based catalysts, the O–O bond in O2 and H2O2 is easily dissociated due to the higher energy sites of Pd, which decreases the selectivity and productivity of H2O2. To address this issue, non-noble metals M (M = Sn, Fe, Co, Ni) were doped into palladium precursors to create a series of yolk–shell structure bimetallic catalysts Pd–M@HCS (H = hollow; C = carbon; S = sphere) with Pd–M as the core and porous carbon as the shell. The results indicated that the catalyst Pd–M@HCS doped with Sn, Fe, Co, and Ni has a weak dissociation ability for O2, and both the adsorption and dissociation ability for H2 are improved. Of these catalysts, the catalyst Pd–Sn@HCS gives the best performance, which is benefited by the suitable Pd–Sn nanoparticle size and the best Pd2+/Pd0 ratio. The influence of the nPd/nSn ratio in the Pd–Sn@HCS system on catalyst performance was further explored, and the findings revealed that Pd–Sn@HCS had the best catalytic activity and stability when the nPd/nSn ratio was 2. The catalyst's H2 conversion, H2O2 selectivity, and productivity were 35%, 97%, and 3961 mmol gPd−1 h−1, respectively. After 10 cycles, the H2O2 productivity of this catalyst remained at 92.1%, which was greater than the H2O2 productivity of the typical Pd-based catalyst Pd/C, which stayed at 37% under the same conditions.
研究领域:
催化
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化学工程
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材料科学
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无机化学
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产品关联
DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2024
·
IF 8.4
Ting He,Shuang Yao,Dejian Chen,Zhaoyun Sun,Xiaoyun Wang,Keyi Wang,Jiangwei Chen,Qingguo Li,Rizhi Chen,Yawei Wang,Zhaoliang Cui
Membrane oxygenator performs lung function in the Extra-corporeal Membrane Oxygenation (ECMO) system. In the clinical use, to ensure the balance of gas exchange of patient’s body, the gas-blood exchange membrane is required to possess CO 2 /O 2 selectivity, which is suggested to be in the range of 10-12. In our work, the molecular dynamics simulation results displayed that the amino-functionalized Zr-MOFs provides fast transport channels for CO 2 molecules because of the enhancement of the adsorption and diffusion ability for CO 2 . Therefore, we chose organic ligands with abundant CO 2 -philic groups to synthesize target amino-functionalized Zr-MOFs, and then dispersed them into medical-grade PDMS solution to study the separation performance of CO 2 /O 2 . On the basis of constructing anti-leakage coating layer, biomimetic gas channels were designed to increase the clearance rate of CO 2 . Experimental results exhibited that the CO 2 /O 2 selectivity of (NH 2 ) 2 -UiO-66/PDMS MMM was as high as 11.19, which was basically consistent with the simulation results. The obtained amino-functionalized Zr-MOF/PDMS coating layer displayed favorable biocompatibility and biosafety. Meanwhile, the construction of biomimetic channel solves the difficult problem of CO 2 removal in PMP membrane, which verifies the feasibility of applying porous materials to gas-blood exchange membranes in the ECMO system.
研究领域:
材料科学
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生物医学工程
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分子动力学模拟
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膜技术
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产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2019
·Vol. 44
·期 5
·1795-1805
·
IF 3.069
Hao Liu,Xiaodong Zhu,Rui Han,Yuxue Dai,Yuanling Sun,Yanna Lin,Dandan Gao,Xueying Wang,Chuannan Luo
Study of the degradation mechanism of the Cu2O/g-C3N4 p–n heterojunction is very challenging and important for the preparation and practical applications of the g-C3N4 photocatalyst in controlling water pollution. Therefore, the Cu2O/g-C3N4 p–n heterojunction was designed and prepared successfully and the mechanism of enhanced visible-light photocatalytic activity was proposed. The morphology and structure of the synthesized materials were characterized by using SEM, TEM, FT-IR and XPS. And the optical and electrical properties of the materials were studied by measuring DRS, the photocurrent density and the Mott–Schottky curve. The results showed that the g-C3N4 photocatalyst is coated on the surface of Cu2O to form a tight heterojunction, which facilitates the separation and migration of photogenerated carriers, and the quantum yield of the Cu2O/g-C3N4 composite photocatalyst was 3–7 times higher than that of the single component. It has been shown that the built-in electric field formed at the heterojunction interface can effectively separate photogenerated electrons and holes. The photocatalytic performance of the material was evaluated by the photocatalytic degradation of tetracycline (TC) under visible light. The maximum degradation rate of Cu2O/g-C3N4 for TC could reach over 90% in 90 min, and the degradation rate of the single component is more than doubled. Simultaneously, the TOC tests monitored the mineralization of TC up to 83.4%, and the active substances in the reaction process were determined to be ˙O2− and h+ through free radical trap experiments and ESR tests. This work shows that the construction of an internal electric field has greatly improved the photocatalytic performance of g-C3N4. The Cu2O/g-C3N4 p–n heterojunction has good degradation ability toward tetracycline and is a good tetracycline-type wastewater treatment material.
研究领域:
材料科学
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环境科学
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光化学
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产品关联
DOI
高影响因子
Science Advances
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2017
·Vol. 3
·期 6
·
IF 0
Pengwei Wang,Guofeng Zhao,Yu Wang,Yong Lu
Oxidative coupling of methane (OCM) is a promising method for the direct conversion of methane to ethene and ethane (C2 products). Among the catalysts reported previously, Mn2O3-Na2WO4/SiO2 showed the highest conversion and selectivity, but only at 800° to 900°C, which represents a substantial challenge for commercialization. We report a TiO2-doped Mn2O3-Na2WO4/SiO2 catalyst by using Ti-MWW zeolite as TiO2 dopant as well as SiO2 support, enabling OCM with 26% conversion and 76% C2-C3 selectivity at 720°C because of MnTiO3 formation. MnTiO3 triggers the low-temperature Mn2+↔Mn3+ cycle for O2 activation while working synergistically with Na2WO4 to selectively convert methane to C2-C3. We also prepared a practical Mn2O3-TiO2-Na2WO4/SiO2 catalyst in a ball mill. This catalyst can be transformed in situ into MnTiO3-Na2WO4/SiO2, yielding 22% conversion and 62% selectivity at 650°C. Our results will stimulate attempts to understand more fully the chemistry of MnTiO3-governed low-temperature activity, which might lead to commercial exploitation of a low-temperature OCM process.
研究领域:
化学工程
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催化
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能源化学
✓ 已验证
产品关联
DOI
PubMed
MICROPOROUS AND MESOPOROUS MATERIALS
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2022
·
IF 5.876
Ning Zhang,Xiaofeng Ning,Jia Chen,Jianming Xue,Gongxuan Lu,Hongdeng Qiu
The development of TiO 2 -based composites with a broad light response and outstanding photocatalytic performance is very important for the removal of antibiotics. In this work, we prepared a series of new porous graphene (PG)/TiO 2 nanocomposites formed the different highly reactive interface within confined space via a partial combustion strategy using TiCl 4 as the Ti source. The as-prepared PG/TiO 2 exhibited the simultaneous effect of incredible adsorptivity and photodegradation performance toward tetracycline (TC) antibiotic under UV and visible light in contrast to conventional PG/TiO 2 , pure TiO 2 (P25) and PG. Optimization experiments showed that PG/TiO 2 -4% had the optimal removal performance among all the nanocomposites. The removal rate of TC reached up to 95.5%, which was 15% higher than that of I-PG/TiO 2 and 25% higher than that of P25 within 90 min. The results were credited to (1) the high specific surface area and porous structure of PG, (2) the broad light response range and rapid separation of h + and e − of PG/TiO 2 , and (3) the highly reactive interface between PG and TiO 2 nanoparticles . In addition, active radical trapping experiments indicated that ·O 2 − was crucial to the elimination of TC. This work showed the new potential of PG/TiO 2 nanocomposites for the enhanced photocatalytic performance.
研究领域:
环境科学
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材料科学
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纳米技术
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Energy Materials
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2025
·
IF 5.5
Qiang Li,Chuang Shi,Zhiguang Zhang,Hong Sun,Tian Zhang,Jie Li,Zhichao Xue,Tianyu Zhang,Mingfu Yu,Haotian Chen,Peng Zhou
Li–O2 batteries have attracted great attention due to their extremely high theoretical energy density. However, they suffer from a short cycle life and low capacity in practical applications. These problems stem from the inability to fully decompose the Li2O2 generated during the discharge process. In this study, NiFe2O4 catalysts with two different morphologies, octahedral and microflowers, were prepared by a simple hydrothermal method. The effects of NiFe2O4 cathodes with different morphologies on the performance of Li–O2 batteries were investigated. Theoretical calculations reveal that the overpotentials of the oxygen reduction reaction and oxygen evolution reaction of the battery with NiFe2O4 are 0.52 and 0.65 V, respectively. The results show that the octahedral Super-P/NiFe2O4 cathode exhibits high catalytic activity and shows a large specific surface area and a reasonable pore structure, resulting in the reduction in charge/discharge potential difference. The battery equipped with an octahedral Super-P/NiFe2O4 cathode exhibits the best cycle life of 125 cycles at a current density of 500 mA·g–1 and presents the highest discharge capacity of 9427 mAh·g–1 at a current density of 100 mA·g–1.
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DOI
高影响因子
ELECTROCHIMICA ACTA
·
2023
·
IF 6.6
Congcong Dang,Pu Feng,Sixian He,Liancheng Zhao,Aidang Shan,Ming Li,Lingti Kong,Liming Gao
The design of ultra-stable cathode materials of Li-O 2 batteries with excellent catalytic performance is very important and desirable. However, some problems such as sluggish electrochemical reaction kinetics and unwanted side reactions still remain challenging. Carbon materials own hierarchical porous structure which facilitates mass transport and accommodates discharge products but are not stable enough as cathode of Li-O 2 batteries. Here in, we fabricated a unique NiCo bimetallic phosphide combined with carbon nanotube heterostructure (abbreviated as NiCoP/CNT) by hydrothermal method. Density functional theory (abbreviated as DFT) calculation demonstrates that bimetallic phosphide NiCoP/CNT delivered much better electrical conductivity, greater adsorption to reactants, and more electron transfer with discharge products Li 2 O 2 , compared to monometallic phosphides CoP and Ni 2 P. Therefore, NiCoP/CNT based cathode displayed low overpotential of 0.87 V at current of 100 mA g −1 with a fixed specific capacity of 1000 mAh g −1 and run steadily over 150 cycles under high current of 500 mA g −1 with a fixed specific capacity of 1000 mAh g −1 . Furthermore, Ex-situ X-ray Photoelectron Spectroscopy and in-situ differential electrochemical mass spectroscopy proved the existence of intermediate products Li 2-x O 2 . This approach provides a reference for designing and synthesis of bimetallic cathode in Li-O 2 batteries.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
ELECTROCHIMICA ACTA
·
2016
·
IF 4.803
Jingpeng Wang,Chunyu Du,Xing Xu,Xiaoshu He,Geping Yin,Yulin Ma,Pengjian Zuo,Xinqun Cheng,Yunzhi Gao
A facile high-temperature solid phase approach is employed to coat lithium phosphorus oxynitride (LiPON) layer on the concentration gradient Li[Ni 0.73 Co 0.12 Mn 0.15 ]O 2 material with Ni-rich core and Ni-poor surface. X-ray diffraction, scanning electron microscopy, transmission electron microscopy and X-ray photoelectron spectroscopy demonstrate that LiPON forms an even coating with ∼4 nm of thickness on the surface without destroying the bulk structure of Li[Ni 0.73 Co 0.12 Mn 0.15 ]O 2 material. The LiPON-coated concentration gradient Li[Ni 0.73 Co 0.12 Mn 0.15 ]O 2 material exhibits a capacity retention of 87.3% at 25 °C after 1000 cycles and 89.9% at 55 °C after 250 cycles, which is 36.1% and 17.2% higher than that of pristine Li[Ni 0.73 Co 0.12 Mn 0.15 ]O 2 material, respectively, under the same operating conditions. This significantly improved cycling performance is ascribed to the noncrystalline LiPON layer on the surface, which provides a reliable interface protection. The LiPON coating is an effective approach to enhancing the electrochemical performance of electrode materials for lithium ion batteries.
研究领域:
材料科学
·
电化学
✓ 已验证
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
·
能源存储技术
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2018
·
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
·
环境科学
·
化学工程
✓ 已验证
DOI
高影响因子
ENERGY & FUELS
·
2020
·
IF 3.421
Qiongqiong Jiang,Yali Cao,Xiangyu Liu,Hao Zhang,Hui Hong,Hongguang Jin
Chemical looping combustion (CLC) can achieve the benefits of efficient conversion of hydrocarbon fuels and zero-energy CO2 capture using oxygen carriers (OCs) with facilitated oxygen transport properties. The current study details the use of Cu- and Ca-doped lanthanum nickel perovskite-type materials as the OC in CLC processes. By incorporation of lanthanum nickel oxide with copper and calcium, the oxygen storage capacity and average transport rate of La1–yCayCuxNi1–xO3 are up to 7.8 wt % and 0.82 wt % min–1, respectively, during the methane CLC process at 400 °C, whereas undoped LaNiO3 cannot react with methane at a low temperature. Simultaneously, substituted lanthanum nickel oxides can decrease the oxygen transport temperature by about 70 °C compared to undoped lanthanum nickel oxide. X-ray diffraction, Brunauer–Emmett–Teller, and scanning electron microscopy of the samples were characterized in terms of particle properties and morphology to unveil the rational reasons of the high oxygen transport at lower temperatures. The enhancement of the specific surface area and stable porous morphology in La1–yCayCuxNi1–xO3 can both facilitate the oxygen transport in CLC processes. Experiments were executed to investigate the reactivity of the redox materials on the standpoints of oxygen capacity, stability, and regenerability. Hydrogen and methane as the fuels are both considered in this study. La1–yCayCuxNi1–xO3 showed favorable reactivity and stability in the successive redox cycles at low temperatures. These experimental results indicate that La1–yCayCuxNi1–xO3 can facilitate O2– transport and have the potential to be used as the promising OC for low-temperature CLC processes.
研究领域:
能源化学
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材料科学
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化学工程
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环境科学
·
催化化学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2026
·
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
危险品化学品经营许可证（带存储）