ADVANCED FUNCTIONAL MATERIALS
·
2023
·Vol. 33
·期 16
·2214215
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IF 19
Xiaosong Hu,Xinyu Liu,Xin Hu,Chaoyue Zhao,Qingxin Guan,Wei Li
Reverse water-gas shift (RWGS) reaction is the initial and necessary step of CO 2 hydrogenation to high value-added products, and regulating the selectivity of CO is still a fundamental challenge. In the present study, an efficient catalyst (CuZnN x @C-N) composed by Zn single atoms and Cu clusters stabilized by nitrogen sites is reported. It contains saturated four-coordinate Zn-N 4 sites and low valence CuN x clusters. Monodisperse Zn induces the aggregation of pyridinic N to form Zn-N 4 and N 4 structures, which show strong Lewis basicity and has strong adsorption for *CO 2 and *COOH intermediates, but weak adsorption for *CO, thus greatly improves the CO 2 conversion and CO selectivity. The catalyst calcined at 700 °C exhibits the highest CO 2 conversion of 43.6% under atmospheric pressure, which is 18.33 times of Cu-ZnO and close to the thermodynamic equilibrium conversion rate (49.9%) of CO 2 . In the catalytic process, CuN x not only adsorbs and activates H 2 , but also cooperates with the adjacent Zn-N 4 and N 4 structures to jointly activate CO 2 molecules and further promotes the hydrogenation of CO 2 . This synergistic mechanism will provide new insights for developing efficient hydrogenation catalysts.
研究领域:
化学
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催化材料科学
✓ 已验证
产品关联
DOI
高影响因子
Nanoscale
·
2024
·
IF 5.8
Ziyin Yang,Yaqi Kong,Chengcheng Qi
Compared with transition metals with partially occupied 3d orbitals, Zn has a filled 3d10 configuration, which severely restricts electron mobility and hence usually renders Zn2+ intrinsically inactive for electrochemical sensing. Metal single-atom catalysts are a new kind of sensing material. Owing to their unique coordination structure and high atomic utilization rate, metal single-atom catalysts show unique properties, which makes them promising for use in the field of electrochemical sensing. However, whether Zn single atoms are active sites remains to be elucidated. In this study, we prepared nitrogen-doped carbon (NC) materials by pyrolyzing ZIF-8 at high temperatures and reported that when the pyrolysis temperature was 800 °C, many Zn single atoms with Zn-N4 coordination structures remained in the NC material. Even when the pyrolysis temperature is increased to 1000 °C, a small number of Zn single atoms remain, and the coordination structure changes from Zn-N4 to Zn-N3. Furthermore, unexpectedly, both residual Zn single atoms showed electrocatalytic activity for H2O2 reduction. In particular, the electrocatalytic activity was significantly enhanced after the coordination structure was changed from Zn-N4 to Zn-N3. Density functional theory (DFT) calculations indicate that the coordination structure of Zn-N3 optimizes the adsorption and desorption strength of oxygen-containing species in the electrocatalytic reaction process, which lowers the energy barrier of the rate-determining step and increases the detection sensitivity of H2O2 nearly 4.1 times. This study revealed new properties of Zn single atoms for the electrocatalytic reduction of H2O2 and developed a strategy to increase the electrocatalytic activity of metal single-atom catalysts through coordination number regulation, which lays the foundation for the use of Zn single atoms in the field of electrochemical sensing and provides ideas for the design of new highly active sensing materials.
研究领域:
材料科学
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电化学
·
催化科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
·
IF 6.2
Mingna Chu,Kai Cui,Yan Zhou,Xiuzhi Yuan,Wei Qin,Yang Li,Xiaohong Wu
Enhancing the photoreduction of carbon dioxide (CO 2 ) to produce valuable chemicals, such as carbon monoxide (CO), is of significant importance. The bottleneck in developing advanced catalysts lies in the rational design of catalytic centers with efficient CO 2 activation and hydrogen proton production. In this work, palladium nanoparticles (Pd NPs) were successfully modified on UiO-66-NH 2 -Zn SAs (UN-Zn SAs) by a photo-deposition method. The optimized photocatalyst , 4 Pd NPs-UN-0.7Zn SAs, demonstrated exceptional performance in converting CO 2 to CO, exhibiting approximately 1.4-fold and 7.8-fold enhancements compared to UN-0.7Zn SAs and UN, respectively. A combination of time-resolved photoluminescence spectroscopy and electron paramagnetic resonance results unveiled that the introduction of Pd NPs effectively promoted the photogenerated charge separation and facilitated water activation to produce more hydrogen protons. The generated hydrogen protons were subsequently coupled with nearby CO 2 that was activated by Zn SAs, thus achieving the facile water-activation-induced CO 2 reduction process. Theoretical calculations further confirmed that the heterogeneous synergistic effects between Zn SAs and Pd NPs lowered the energy barrier for the rate-limiting step of CO 2 conversion to COOH* , thereby achieving efficient photocatalytic CO 2 reduction reactions. This work provides a new perspective on the development of efficient catalysts for the effective conversion of CO 2 .
研究领域:
化学
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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
Nature Communications
·
2025
·Vol. 16
·期 1
·1-12
·
IF 15.7
Wei Shengjie,Zhu Jiexin,Chen Xingbao,Yang Rongyan,Gu Kailong,Li Lei,Chiang Ching-Yu,Mai Liqiang,Chen Shenghua
Breaking the geometric symmetry of traditional metal-N 4 sites and further boosting catalytic activity are significant but challenging. Herein, planar chlorination engineering is proposed for successfully converting the traditional Zn-N 4 site with low activity and selectivity for CO 2 reduction reaction (CO 2 RR) into highly active Zn-N 3 site with broken symmetry. The optimal catalyst Zn-SA/CNCl-1000 displays a highest faradaic efficiency for CO (FE CO ) around 97 ± 3% and good stability during 50 h test at high current density of 200 mA/cm 2 in zero-gap membrane electrode assembly (MEA) electrolyzer, with promising application in industrial catalysis. At -0.93 V vs. RHE, the partial current density of CO ( J CO ) and the turnover frequency (TOF) value catalyzed by Zn-SA/CNCl-1000 are 271.7 ± 1.4 mA/cm 2 and 29325 ± 151 h -1 , as high as 29 times and 83 times those of Zn-SA/CN-1000 without planar chlorination engineering. The in-situ extended X-ray absorption fine structure (EXAFS) measurements and density functional theory (DFT) calculation reveal the adjacent C-Cl bond induces the self-reconstruction of Zn-N 4 site into the highly active Zn-N 3 sites with broken symmetry, strengthening the adsorption of * COOH intermediate, and thus remarkably improving CO 2 RR activity.
研究领域:
材料科学
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催化化学
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能源化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Small
·
2024
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IF 13
Mengmeng Zhang,Mingzhu Lu,Yimin Gong,Yannan Yang,Junfei Song,Jianing Li,Zhenxia Chen,Yun Ling,Yaming Zhou
Precise integration of diverse therapeutic approaches into nanomaterials is the key to the development of multimodal synergistic cancer therapy. In this work, tadpole-like carbon nanotubes with Fe nanoparticle encapsulated at the head and Zn single-atom anchored on the body (Fe@CNT-Zn) is precisely designed and facilely prepared via one-pot carbonization. In vitro studies revealed the integration of chemotherapy (CT), chemodynamic therapy (CDT), photothermal therapy (PTT), and photodynamic therapy (PDT) in Fe@CNT-Zn as well as the near-infrared light (NIR)-responsive cascade therapeutic efficacy. Furthermore, in vivo studies demonstrated the NIR-triggered cascade-amplifying synergistic cancer therapy in a B16 tumor-bearing mouse model. The results not only showcased the Fe@CNT-Zn as a potential tetramodal therapeutic platform, but also demonstrated a proof-of-concept on metal–organic framework-based “one stone for multiple birds” strategy for in situ functionalization of carbon materials.
研究领域:
生物医学工程
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纳米医学
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肿瘤治疗
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Acta Biomaterialia
·
2024
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IF 9.4
Sheng Dai,Li Yao,Luying Liu,Jiawei Cui,Zhaogui Su,Ansha Zhao,Ping Yang
Diabetic wound treatment continues to be a significant clinical issue due to higher levels of oxidative stress, susceptibility to bacterial infections, and chronic inflammatory responses during healing. We rationally developed and synthesized an ultra-small carbon dots (C-dots) loaded with zinc single-atom nanozyme (Zn/C-dots) with the aim of promoting wounds healing by nanocatalytic treatment, especially targeting its complex pathological microenvironment. Zinc single atoms and C-dots form a dual catalytic system with higher enzymatic activity. Furthermore, the Zn/C-dots nanozyme effectively enters cells, accumulates at mitochondria, and removes excess ROS, protecting cells from oxidative stress damage and limiting the release of pro-inflammatory cytokines, hence reducing inflammation. Zinc can synergistically increase the antibacterial action of C-dots (the effective antibacterial rate of 100 μg/mL Zn/C-dots was above 90%). Unlike traditional C-dots, Zn/C-dots can cause endothelial cell migration and the formation of new blood vessels. In vitro cytotoxicity, blood compatibility, and in vivo toxicity studies of Zn/C-dots show that they are biocompatible. We subsequently utilized the Zn/C-dots nanozymes to treat diabetic rats' chronic wounds for external use, combining them with ROS-responsive hydrogels to create an antioxidative system (H-Zn/C-dots). The hydrogels anchored the Zn/C-dots nanozymes to the wound, allowing for long-term treatment. The results revealed that H-Zn/C-dots can considerably reduce inflammation, accelerate angiogenesis, collagen deposition, and promote tissue remodeling at the diabetic wound site. After 14 days, the wound area had decreased to approximately 9.19%, making it a potential treatment. Statement of significance An ultra-small carbon dot with a zinc single-atom nanozyme was designed and manufactured. Zn/C-dots possess antibacterial, ROS-scavenging, and angiogenesis activities. In vivo , the multifunctional ROS-responsive hydrogel incorporating Zn/C-dots could speed up diabetic wound healing.
研究领域:
纳米技术
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生物医学工程
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伤口愈合
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材料科学
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药学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Functional Materials Letters
·
2024
·
IF 1.2
Hui Wang,Nairan Li
The instability of lithium metal and insoluble discharging products, Li 2 O 2 , has been a formidable challenge that hinders the widespread implementation of lithium-air batteries (LABs). Hybrid electrolyte-based LABs have been proposed as one of the most promising strategies to solve these issues. However, the complex device designs together with a suitable solid electrolyte membrane is one of the key parameters that determine the battery run. Herein, we present a novel approach featuring a three-phase “organic-solid-aqueous” hybrid electrolyte for LABs, incorporating a NASICON-based solid electrolyte and zinc single atoms catalysts. It is clarified that Li 1 . 3 Al 0 . 3 Ti 1 . 7 ( PO 4 ) 3 (LATP) shows much-enhanced stability compared with the pulverization of Li 1 . 3 Al 0 . 3 Ge 1 . 7 ( PO 4 ) 3 (LAGP) by the reduction of Ge upon the Li + transport across. Combined with the bifunction of Zn SAs/CNF catalysts in ORR/OER, the 4 e − pathway has been proven to be established as a primary contributor to the battery’s high efficiency, which can well run over 100 h in the ambient air at room temperature. These innovative methodologies and insights hold promise for advancing the practical application of safe LABs and may extend to various air battery technologies.
研究领域:
储能技术
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电化学
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材料科学
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电池技术
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固态电解质
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Junyao Song,Haoyu Chen,Yaqian Lv,Wanqun Yang,Fenglang Zhang,Tianyi Wang,Danping Liu,Yingshan Qu,Lei Han,Jun Fu,Xiaoying Kong
Single-atom catalysts (SACs), characterized by atomically dispersed single metal atoms, provide superior antibacterial properties over common nanozyme materials due to their satisfactory catalytic activity. However, when used for the treatment of biofilm-infected wounds, SACs are still unable to effectively solve severe microbial infection due to the insufficient supply of reactive oxygen species (ROS). Herein, a new hybrid nanozymes consisting of Zn single-atom catalysts and copper peroxide (Zn SACs@CuO 2 ) were prepared to realize the upgrading of ROS generation and the combination of photothermal/chemodynamic (PTT/CDT) therapy for biofilm-infected wound. Specifically, CuO 2 exhibited not only excellent photothermal property, but also H 2 O 2 -producing and Fenton-like catalytic activities, which assisted Zn SACs to accelerate the ·OH conversion of endogenous and exogenous H 2 O 2 . Compared with single antimicrobial strategies of Zn SACs, Zn SACs@CuO 2 hybrid nanozymes exhibited stronger therapeutic effects of biofilm destruction, immune activation and inflammation improvement. In conclusion, this work developed a hybrid single atom nanozyme material with for efficient biofilm-infected wound healing.
研究领域:
纳米技术
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材料科学
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生物医学工程
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伤口愈合
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抗菌治疗
✓ 已验证
产品关联
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2025
·
IF 19
Shuofeng Li,Fangfang Wang,Chenhuan Wang,Lin Hao,Ningzhao Shang,Pengbo Zhang,Yawen Zhang,Nuo Xiao,Yaai Kang,Jin Liu,Shutao Gao,Chun Wang,Zhi Wang,Qiuhua Wu
Single-atom nanozyme (SAZ) with peroxidase-like activity has attracted great attention in point-of-care (POC) diagnostic, but the use of unstable H 2 O 2 in peroxidase catalytic reactions often leads to low detection accuracy. Thus, developing SAZ with high oxidase (OD)-like activity to construct RNA sensing systems independent of H 2 O 2 is imperative for improving accuracy. Herein, a novel strategy to fabricate boron-nitrogen co-doped zinc SAZ (ZnBNC-SAZ) with excellent OD-like activity by carbonizing Zn based zeolitic boron imidazolate frameworks is reported. The electron deficient B in imidazolate ligand can form Zn─N─B bond in situ during high temperature pyrolysis, which can regulate the electronic structure of Zn and further upshift the d-band center of Zn to improve the OD-like activity. With ZnBNC-SAZ as signal generator, a new method for sensitive RNA detection is developed by combining CRISPR/ cas13 system with terminal deoxynucleotidyl transferase-induced DNA extension reaction. The limits of detection for RNAs are as low as 20 aM. The proposed biosensor is adaptable to a lateral-flow-based readout and is universally applicable for sensing various RNAs by programming the guide RNA. Importantly, the proposed biosensor can monitor the cellular differentiation and identify patients with cervical carcinoma, showing great potential for application in facile POC diagnosis.
研究领域:
纳米技术
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生物化学
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分子生物学
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医学诊断
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生物医学工程
✓ 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）