CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Chao Wang,Long Kuai,Wei Cao,Harishchandra Singh,Alexei Zakharov,Yuran Niu,Hongxia Sun,Baoyou Geng
The preparation of oxygen reduction reaction (ORR) and hydrogen evolution reaction (HER) catalysts with high activity, stability and low platinum loading has always been the focus of research. The single-atom platinum supported catalyst greatly improves the utilization of platinum, but the catalytic activity and selectivity are greatly affected by the platinum coordination environment, and the preparation of the material is difficult. Doping base metals to adjust the electronic structure of platinum is an effective strategy to improve catalyst performance. In this work, copper-platinum alloy nanoparticles were loaded on N-doped porous carbon via a targeted route guided by highly dispersed Cu atoms derived from MOF. The product C-ZIF-CuPt has high activity and high stability ORR, HER bifunctional catalytic performance, which is better than commercial Pt/C (20 wt%). The Pt activity in C-ZIF-CuPt is 4.4 times (ORR) and 6.7 times (HER) than Pt/C. Spectromicroscopic determinations unveiled that strong interactions between carbon carrier and the CuPt alloys contribute to the overall stabilities. DFT calculations show that Cu doping can increase the d-band center of Pt, reduce the ORR overpotential, and the activation energy barrier to water molecules, which is beneficial to ORR and HER catalysis. Under the same carrier conditions, the performance of sub-nano (single atoms, clusters) platinum-supported catalysts (C-ZIF-Cu-Pt) is inferior to C-ZIF-CuPt. This further shows that platinum alloying can effectively improve the performance of the catalyst.
研究领域:
材料科学
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催化化学
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能源科学
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DOI
高影响因子
Small
·
2021
·Vol. 17
·期 43
·2101393
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IF 13.281
Shiyin Zhao,Yangke Long,Yiping Su,Shubin Wang,Zuotai Zhang,Xuanjun Zhang
Antibiotics discharge has been a critical issue as the abuse in clinical disease treatment and aquaculture industry. Advanced oxidation process (AOPs) is regarded as a promising approach to degrade organic pollutants from wastewater, however, the catalysts for AOPs always present low activities, and uncontrollable porosities, thus hindering their further wider applications. In this work, an aliovalent-substitution strategy is employed in metal-organic framework (MOF) precursors assembly, aiming to introduce Co(II/III) into Ce-O clusters which could modify the structure of the clusters, then change the crystallization, enlarge the surface area, and regulate the morphology. The introduction of Co(II/III) also enlarges the pore size for mass transfer and enriches the active sites for the production of sulfate radicals (SO 4 • − ) in MOF-derived catalysts, leading to excellent performance in antibiotics removal. Significantly, the CeO 2 •Co 3 O 4 nanoflowers could efficiently enhance the generation of sulfate radical SO 4 • − and promote the norfloxacin removal efficiency to 99% within 20 min. The CeO 2 •Co 3 O 4 nanoflowers also present remarkable universality toward various antibiotics and organic pollutants. The aliovalent-substitution strategy is anticipated to find wide use in the exploration of high-performance MOF-derived catalysts for various applications.
研究领域:
环境科学
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材料科学
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化学工程
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催化
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废水处理
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2024
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IF 5.8
Guizhen Liu,Shanshan Zhang,Yutian Cai,Yongzhi Cheng,Yingli Zhu,Pingan Chen,Hui Luo,Xiangcheng Li,Fu Chen
Flexible manipulations of morphology and composition have been considered as an art to achieve excellent microwave absorption performance for absorbers derived from metal-organic frameworks (MOFs). In this work, a strategy combining ligand-exchange induced hollow engineering and high-temperature one-step sulfuration has been proposed to fabricate the Co 9 S 8 /Co@N, S dual-doped carbon-based absorbers with tailored solid, yolk-shelled and entirely hollow polyhedral morphologies. The progressive hollow engineering not only enables composition control in the sulfuration process, but also endows the proposed absorbers with superior microwave absorption capacity due to the enhanced conductivity loss and Maxwell-Wagner polarization as well as optimized impedance matching. The yolk-shelled Co 9 S 8 /Co@N, S dual-doped carbon-based composite achieves a broad effective absorption bandwidth of 5.13 GHz at 1.88 mm with 20 wt% loading and realizes a minimum microwave loss of − 51.78 dB @ 11.63 GHz with 2.37 mm. This work reveals that the joint strategy of ligand-exchange induced hollow engineering and gas-solid reactive thermal process is an effective path to construct high-efficient lightweight multi-interfacial microwave absorbers for addressing the electromagnetic pollutions.
研究领域:
材料科学
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电磁学
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产品关联
DOI
高影响因子
JOURNAL OF NANOBIOTECHNOLOGY
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2026
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IF 15
Zhang Yiling,Li Yu,Lu Jiayu,Qin Xin,Wang Zixin,Cai Aojie,Fan Ling,Jin Ronghua,Xie Yandong
To address the therapeutic limitations and metabolic toxicity associated with conventional nanocarriers, a nanostructure using an “MOF-in-MOF” strategy was engineered. The comprises an olsalazine (Olsa)-based copper metal-organic framework (Olsa-MOF) that integrates intrinsic anti-inflammatory properties and enhanced chemodynamic performance. This Olsa-MOF template is integrally enveloped by a tumor microenvironment-responsive TK-based Cu-MOF layer, which demonstrates exceptional photothermal properties. Subsequent surface functionalization with dopamine-grafted hyaluronic acid (DOPA-HA) endows active targeting ability, yielding the final nanocomposite termed Olsa@TK-Cu@HA. Olsa@TK-Cu@HA not only overcomes the limitations of conventional nanocarriers but also offers a novel strategy to enhance the therapeutic efficacy of photothermal therapy (PTT) and chemodynamic therapy (CDT) through targeted modulation of the COX-2/PGE2 inflammatory axis. The Olsa@TK-Cu@HA demonstrates a superior photothermal conversion efficiency (26.8%) and robust reactive oxygen species (ROS) generation, along with pH-responsive release of Olsa. In vitro evaluation demonstrated that Olsa@TK-Cu@HA exerts tumor-selective cytotoxicity, showing 3.5-fold higher potency against cancer cell. Moreover, Olsa@TK-Cu@HA effectively induces immunogenic cell death (ICD), as evidenced by increased extracellular ATP efflux (5.06-fold elevation) and CRT exposure. Concurrently, it downregulates the COX‑2/PGE2 axis to relieve immunosuppression in the tumor microenvironment and suppresses PD‑L1 expression. This coordinated action amplifies ICD‑mediated antitumor immunity, leading to a tumor regression rate of 84.0% in vivo. By integrating precision targeting, stimulus-responsive drug release, and immunometabolic reprogramming, this work moves beyond conventional treatment paradigms and establishes an innovative platform for next‑generation cancer therapy. Graphical The alternative text for this image may have been generated using AI.
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DOI
PubMed
高影响因子
ACS Catalysis
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2022
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IF 13.7
Wei Qu,Zhuoyun Tang,Hailin Wen,Manhui Luo,Tao Zhong,Qiyu Lian,Lingling Hu,Shuanghong Tian,Chun He,Dong Shu
High-performance and robust catalysts act as core drivers for catalytic ozonation to eliminate gaseous sulfur-containing volatile organic compounds (VOCs). Herein, nitrogen-doped carbon nanotubes embedded with Co species (Co@NCNT) are synthesized by thermolysis of a ZIF-67/melamine mixture. The carbon-confinement effects in Co@NCNT not only improve the stability of Co species but also regulate the electronic structure of Co─C bonds, consequently synergistically improving the catalytic ozonation performance. The experimental results indicate that the Co@NCNT catalyst could still remove ∼86% of odorous methyl mercaptan (CH3SH) after running for 60 h at 25 °C under an initial concentration of 50 ppm CH3SH and 40 ppm ozone, relative humidity of 60%, and space velocity of 600,000 mL h–1 g–1, outdistancing reported values under comparable reaction conditions. Detailed characterization and theoretical simulations reveal that the electronic metal–support interaction of Co─C bonds in Co@NCNT significantly adjusts the electronic structure of Co species, thereby promoting ozone-specific adsorption/activation to convert the surface atomic oxygen (*Oad) and ·OH/1O2/·O2–. Also, the electrons obtained from CH3SH in the electron-poor center transferred through the C─Co bond bridge to maintain the redox cycle of ≡Co0/2+ → ≡Co3+ → ≡Co0/2+ and realize the efficient and stable removal of CH3SH into CO2/SO42–/H2O. This work demonstrates that MOF-derived materials with tunable electronic structures achieve the stable removal efficiency for gaseous sulfur-containing VOCs via electron transfer trade-offs and provide potential candidate catalysts for the application of air purification.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2025
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IF 21.1
Juntian Li,Zhiling Xu,Junhui Zhou,Xinjie Wang,Jiachun Cao,Qianyu Li,Teng Wang,Juan Li,Didi Li,Zhimin Ao
Designing multifunctional catalysts for low-temperature co-oxidation of volatile organic compounds (VOCs) and CO is challenging, as conventional catalysts cannot simultaneously achieve VOCs activation and CO poisoning resistance below 200 °C—where CO preferentially adsorbs and severely inhibits VOCs oxidation. Herein, we proposed a density functional theory (DFT)-guided atomic engineering strategy integrating d-band center modulation and adsorption energy screening to construct metal-organic frameworks (MOFs)-hosted Au-Pt single-atom alloys (SAAs). By leveraging the coordination confinement of UiO-66 to stabilize Au-Pt SAAs sites, the optimized Au-Pt SAAs/UiO-66 catalyst achieved exceptional performance in co-oxidation of toluene and CO, attaining 90 % toluene conversion at 160 °C with robust stability under CO-poisoning conditions. Mechanistic studies and DFT calculations revealed that atomically dispersed Au sites induced Pt δ− -Au δ+ charge polarization on Pt nanoparticles charge polarization via interfacial electron transfer, weakening CO adsorption while enhancing toluene activation through dual-pathway mechanisms (Eley-Rideal and Langmuir-Hinshelwood) mechanisms. This synergy decouples the traditional trade-offs between activity and stability, offering a 4.7-fold higher turnover frequency than conventional Pt catalysts. Our work established a paradigm for electronic cooperativity in MOF-hosted SAAs, providing atomic-level insights into the design of multifunctional catalysts for environmental remediation.
研究领域:
催化
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材料科学
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环境化学
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理论化学
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纳米技术
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产品关联
DOI
高影响因子
JOURNAL OF SOLID STATE CHEMISTRY
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2025
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IF 3.5
Zhou-Cao Ye,Jie Liu,Jie Duan,Wei-Li Zhai,Xian Wang,Qing Li,Wei Zhu
Photocatalytic elimination of highly toxic Cr 2 O 7 2− and stubborn reactive dyes requires photocatalysts to exhibit both robust oxidation and reduction capabilities. However, most single MOFs must utilize ultraviolet light and are incapable of concurrently providing sufficiently negative LUCO and positive HUCO potentials. In the current contribution, a water-stable In-MOF featured by typical n-type semiconductor was assembled and subsequently integrated with the in-situ growth In 2 S 3 to construct a novel In 2 S 3 /In-MOF binary heterojunction. Notably, the intrinsic LUCO (−0.43 eV, vs. NHE) and HOCO (2.77 eV, vs. NHE) energy levels of deployed In-MOF exhibit a suitable band dislocation with In 2 S 3 's CB (−0.85 eV, vs. NHE) and VB (1.43 eV, vs. NHE) potentials. And this integration facilitates the establishment of an S-Scheme carrier transfer mechanism, effectively inhibiting carriers recombination and ensuring the efficient utilization of the robust redox abilities offered by In 2 S 3 's CB and In-MOF's HOCO. Under the driven of a low-energy xenon lamp, In 2 S 3 /In-MOF's optical-electrical properties involving photosensitiveness, photocurrent intensity and interface resistance have been notably improved. M55, with a feed mass ratio of In-MOF to In 2 S 3 at 5 : 5, achieved a 99.9 % reduction efficiency for Cr(VI) within 80 min, degradation efficiencies of 77 % and 82 % for reactive dyes RB21 and RR2 within 12 h, respectively. Its reaction kinetics have increased by 8.79, 17.82 and 14.55 times compared to the pristine In-MOF, and by 1.66, 4.60 and 17.57 times relative to pure In 2 S 3 . This contribution offers a viable avenue for designing novel MOFs-based photocatalysts, which possess robust reducing and oxidizing capabilities, to address some intractable water pollution issues.
研究领域:
环境科学
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材料化学
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光催化
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水处理
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半导体物理
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产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
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2024
·
IF 6.3
Jiapeng Wang,Xinpeng Chen,Hua-Bin Yuan,Lili Xing,Desheng Sha,Aijing Li,Guoqiang Chen,Tieling Xing
Metal-organic frameworks (MOFs) find wide-ranging applications owing to their adjustable structures, diverse compositions, and large specific surface area. In this work, MOFs materials were grown in situ on carbon cloth, yielding self-supported electrodes V O -(Fe,Co) 3 O 4 @CC rich in oxygen vacancies through a simple high-temperature annealing treatment utilizing NaBH 4 as an etchant. Thus the resulting self-supported electrode V O -(Fe,Co) 3 O 4 @CC exhibited excellent oxygen evolution reaction (OER) performance, achieving an overpotential of merely 288 mV at 10 mA cm −2 , along with a low Tafel slope of 31.39 mV dec -1 , and demonstrating robust long-term activity and stability. In addition, a liquid zinc-air battery was assembled utilizing the prepared V O -(Fe,Co) 3 O 4 @CC as an air cathode, achieving a high open-circuit voltage of 1.46 V and a high peak power density of 89.06 mW cm −2 , and it maintained excellent cycling stability during cyclic charging and discharging (with a current density of 2 mA cm −2 ) over a 32 h period. Meanwhile, the self-supported electrode V O -(Fe,Co) 3 O 4 @CC served as an air cathode for assembling an all-solid-state flexible zinc-air battery (ZAB), demonstrating a high peak power density (38.21 mW cm −2 ) and exhibiting favorable cycling stability. This experiment offers insights into the potential application of MOF-derived electrocatalysts in water decomposition and zinc-air batteries.
研究领域:
材料科学
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电化学
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能源存储与转换
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产品关联
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2018
·Vol. 28
·期 35
·1802830
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IF 13.325
Huiyuan Zhang,Qian Li,Ruiling Liu,Xinke Zhang,Zhonghao Li,Yuxia Luan
Zeolitic imidazolate framework-8 (ZIF-8) is an attractive metal organic framework (MOF) in drug delivery. Strong interaction between drugs and ZIF-8 is essential for high drug loadings through in situ construction of MOFs. However, only limited drugs with unique functional groups ( COOH, SO 3 H, et al.) can interact with ZIF-8 and be encapsulated satisfactorily so far. Drugs without these functional groups are difficult to be loaded due to the lack of strong interaction. Herein a versatile prodrug strategy is proposed to solve the problems encountered by MOFs. Cytarabine (Ara) is chosen as a model drug since it cannot be loaded in ZIF-8 satisfactorily by itself. New indocyanine green (IR820) is utilized to bond with Ara for the formation of prodrug (Ara-IR820) and endows the prodrug with fluorescence imaging-guided chemo-photothermal therapy, in which sulfonic groups strengthen the interaction between prodrug and ZIF-8. This prodrug loaded ZIF-8 is further functionalized with hyaluronic acid (HA) to result in active-targeting HA/Ara-IR820@ZIF-8 nanoparticles. The in vitro and in vivo results demonstrate its excellent visual cancer therapy with tumor-targeted and pH-responsive release behavior. This design offers a new concept to solve the drug loading problem of MOFs, exhibiting a flexible strategy to expand the biomedical applications of MOFs.
研究领域:
药物递送
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生物医学工程
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癌症治疗
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Xiaohai Yan,Yuning Zhao,Gengan Du,Qi Guo,Hong Chen,Qian He,Qiannan Zhao,Huanfeng Ye,Jianlong Wang,Yahong Yuan,Tianli Yue
Tools to detect low molecular weight mycotoxin patulin (PAT) are urgently needed because of its harm to human health. Here, we report a simple, effective, and sensitive fluorescent aptasensor based on sulfur quantum dots encapsulated in MOF-5-NH 2 ( [email protected] 2 ) and self-cycling catalyzed hairpin assembly (scCHA) for the detection of PAT in apple juice. The [email protected] 2 synthesized by a “bottle-around-ship” solvothermal method works as a fluorescent probe and offers enhanced fluorescence intensity and good water-solubility versus MOF-5-NH 2 due to the encapsulation of water-soluble SQDs . Meanwhile, the scCHA designed by the two DNA hairpins is initiated after the formation of PAT/aptamer, which further recycles PAT to effectively capture multiple fluorescence probes ( [email protected] 2 ) and amplify the detection signal. Attributed to the synergistic effect between the strong fluorescence intensity of [email protected] 2 and the efficient PAT utilization of scCHA, the fluorescent aptasensor exhibits high sensitivity with detection limits as low as 0.753 pg/mL. The system has satisfactory specificity, anti-interference, and reproducibility (RSDs of intra-assay and inter-assay were 3.24% and 8.60%, respectively). The recoveries in apple juice were between 89.03% and 107.67%, which were with good consistency versus high-performance liquid chromatography (HPLC). These data collectively show that the developed fluorescent aptasensor has a good practical application value.
研究领域:
分析化学
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纳米技术
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食品安全
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）