Journal of Environmental Chemical Engineering
·
2025
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IF 7.2
Shujie Liang,Jiaxin Lv,Yishun Wang,Hong Deng
The development of efficient and stable single-atom catalysts (SACs) for CO 2 photoreduction is a persistent challenge. This study reports the successful preparation of SACs by incorporating isolated Ni atoms into carbon nanorods through a low-temperature calcination process using nickel bis(dimethylglyoximate) complexes. These Ni atoms, maintaining their original coordination environments, can facilitate charge separation, and enhance CO 2 adsorption and activation. The optimized catalyst exhibits a CO formation yield of 24.4 µmol with ∼96 % selectivity in high-purity CO 2 , outperforming both the precursor and pure carbon. Additionally, the Ni SACs showed strong catalytic selectivity in diluted CO 2 conditions, with selectivity rates of 82.57 %, 80.35 %, and 61 % at 0.1, 0.05, and 0.01 atm, respectively. This work provides critical insights for designing efficient visible light-responsive CO 2 photoreduction catalysts at the atomic level.
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
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
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IF 9.965
Meichun Qin,Shiying Fan,Xinyong Li,Moses O. Tade,Shaomin Liu
Electroreductive C O coupling provides a prospective strategy for biomass derivative upgrading via reducing the number of oxygen-containing functional groups and increasing their molecular weight. However, exploring superior electrocatalysts with effective reactivity and high selectivity for target products are still a challenge. In this work, single atom Au surface derived NiMn 2 O 4 (SACs Au−NiMn 2 O 4 ) spinel synergetic composites were fabricated by a versatile adsorption-deposition method and applied in electroreductive self-coupling of benzaldehyde to dibenzyl ether . The SACs Au–NiMn 2 O 4 spinel synergetic composites enhanced electroreductive coupling of benzaldehyde, significantly improved the yield and selectivity of dibenzyl ether. Systematic characterizations and density functional theory calculation revealed that atomically dispersed Au occupied surface Ni 2+ vacancies, which played a dominated role in C O coupling of benzaldehyde. Detailed calculation results showed that benzaldehyde preferred to adsorb on Ni octa-hedral sites of NiMn 2 O 4 spinel synergetic structure, single atom Au surficial derivation over NiMn 2 O 4 further reduced the adsorption energy (E ads ) of benzaldehyde on SACs Au−NiMn 2 O 4 , thus the C O coupling of benzaldehyde to dibenzyl ether was promoted. Moreover, single atom Au surficial derivation lowered the energy barrier of rate-determining step, facilitated the formation of dibenzyl ether species. Our work also paves an avenue for rational design single atom materials using spinel as support.
研究领域:
化学
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材料科学
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DOI
PubMed
高影响因子
APPLIED CATALYSIS A-GENERAL
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2025
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IF 4.8
Lu Cheng,Xingtao Ren,Shiyao Lu,Dameng Gao,Jing Yue
Regulating the hydroformylation capacity of heterogeneous catalysts is essential for efficiently converting higher olefins into aldehydes. In this study, a magnetic single-atom rhodium-cobalt-based catalyst (RhCo SACs) was synthesised by modifying Fe 3 O 4 with polymerised carbon nitride. Maintaining a constant metal single-atom loading, the catalytic activity in 1-dodecene hydroformylation was modulated by adjusting the type of N species in the support. The distribution of single atoms and valence states was characterised. At the same time, density functional theory (DFT) calculations were conducted to evaluate substrate binding energies and reaction-free energy barriers, providing insights into reaction mechanisms and pathways. The RhCo-pyridinic N configuration lowered the Gibbs free energy of the rate-determining and hydrogenation steps, enhancing substrate reaction activity. Compared to RhCo-graphitic N, RhCo-pyridinic N demonstrated superior performance, achieving a 1-dodecene conversion rate of 98.3% and aldehyde selectivity of 98.6%. Furthermore, the catalyst was magnetically recovered without loss of activity or mass and maintained stable performance over 10 reuse cycles. These findings present a novel and efficient strategy for the precise design of magnetic single-atom catalysts with potential practical applications in the hydroformylation of high-carbon olefins.
研究领域:
催化化学
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材料科学
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理论计算化学
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DOI
高影响因子
COLLOIDS AND SURFACES B-BIOINTERFACES
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2022
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IF 5.999
Ruigeng Yang,Yueru Wei,Mengyang Zhao,Mengxiao Shi,Yongxing Zhao,Pengchao Sun
The abuse of antibiotics has led to the emergence of multidrug-resistant bacterial strains worldwide, which greatly threatens human health. In the present work, we developed single-atom catalysts (SACs) with atomically dispersed Fe as catalytic sites (Fe-SACs) to combat multidrug-resistant bacteria by elevating cellular reactive oxygen species (ROS). Our intensive studies confirmed that Fe-SACs were successfully prepared and exhibited excellent catalase (CAT)-, oxidase (OXD)-, and peroxidase (POD)-like activities. To enhance water dispersibility, biosafety and the interactions between the nanodrugs and gram-positive bacteria, phenylboronic acid group-functionalized carboxylated chitosan (CCS-PBA) was coated on the surface of Fe-SACs to yield [email protected] for in vitro and in vivo studies. The synergistic catalytic activity and photothermal activity of [email protected] effectively overcame multidrug-resistant bacterial strains ( MRSA) in vitro and significantly accelerated wound healing in vivo , suggesting the great potential of SACs to overcome infectious disease caused by multidrug-resistant bacteria.
研究领域:
纳米技术
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细菌学
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材料科学
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生物医学工程
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药学
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DOI
PubMed
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
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2024
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IF 8
Yuehan Zhang,He Zhang,Xiaoxuan Sun,Panpan Zhao,Junfeng Zhai,Shaojun Dong
Chemical oxygen demand (COD) is a crucial parameter in assessing water quality. Due to the improved public awareness of environmental protection, the rapid, eco-friendly, and cost-effective methods for COD measurement are highly desired. This work proposes a new self-powered COD sensor (SPCS), based on a photocatalytic fuel cell composed of a FeN 5 single-atom nanozymes (FeN 5 SACs)/ITO cathode and a TiO 2 nanotube arrays (TiO 2 NTAs)/Ti photoanode. Because organic compounds are able to be involved as anodic fuels, the detection of COD with the SPCS could be achieved by simply measuring the deviation in short circuit current. The COD detection range is determined to be from 0.5 to 49.4 mg/L, with the limit of detection of 1.38 mg/L. The SPCS possesses satisfactory anti-interference ability against anions including Cl - and SO 4 2- , and high stability even after 60-day storage. For real sample analysis, satisfactory reproducibility (RSD < 6 %), and low relative error (2.48–6.52 %) have been obtained. Besides, the sensor offers the advantages of cost-effectiveness, environmental friendliness, and fast response (< 1 min). Consequently, the SPCS could be regarded as a promising candidate for the sensing of COD.
研究领域:
环境科学
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分析化学
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DOI
高影响因子
INTERNATIONAL JOURNAL OF FOOD SCIENCE AND TECHNOLOGY
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2022
·Vol. 58
·期 5
·2236-2246
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IF 3.612
Xiaoyang Liu,Jiatong Sun,Yue Li,Xuening Yu,Fawen Yin,Deyang Li,Pengfei Jiang,Yoshimasa Nakamura,Dayong Zhou
Summary Recently, food-derived peptides were frequently studied and used as metal ion chelator against negative effects of trace element absorption induced by various human gastrointestinal environments. In this study, the scallop mantle hydrolysates (SMHs) were produced and characterised to study their intestinal promotion of zinc absorption. During production of hydrolysates, the results of degree of hydrolysis (DH) and proteins solubility suggested that the alcalase was suitable for the production of peptides from scallop mantle proteins where the chelating conditions were settled (30 °C, 10 min and 3 mg mL −1 ). The molecular distribution of SMH was mainly 1–5 kDa and chelation of zinc with SMH (involved in carboxyl and amine group of SMH) triggered no significant alteration on the secondary structure of SMH. Zinc morphologically altered the surface structures of SMH. Moreover, SMH could successfully carry and transport zinc while the fluorescence staining indicated free zinc accumulated inside the tissue of everted rat sacs. Finally, several representative transported peptides (intact or cleaved) were identified, such as FTGEPGPSGPT, AINDPFIDL and ALPHAILRI. This study provided a theoretical basis for the investigation of absorption of marine animal-derived peptides as zinc carriers.
研究领域:
食品科学
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营养学
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生物化学
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DOI
高影响因子
ADVANCED MATERIALS
·
2025
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IF 26.8
Haiyang Zhang,Yan Yang,Jianming Zhao,Hanjun Yang,Ying Lu,Yihuan Xie,Shuo Yao,Zhaoyang Chu,Changjian Huang,Zengqi Huang,Mingbin Zhou,Qixin Wan,Qi Li,Tianxiang Zhao,Qianying Lin,Xia Yang,Rui Guo,Zhihua Xiong,Xiaotian Hu
Self-assembled monolayers (SAMs) serve as the hole-transporting layer (HTL) in perovskite solar cells, yet their instability on indium tin oxide (ITO) substrates poses a challenge in practical. The typical SAMs are susceptible to solvents during the perovskite layer deposition process which can result in being washed or dislodged, thereby impeding the formation of a dense SAM. Here, a novel guanidine-modified polyurethane siloxane elastomers is synthesized to enhance the anchoring capability of SAMs on ITO, which exhibits strong interactions with [2-(3,6-dimethoxy-9H-carbazol-9-yl)ethyl] phosphonic acid (MeO-2PACz) SAMs, to co-construct a self-assembled composite structure (SACS). By utilizing this anchor strategy, the weakly bonded MeO-2PACz adhering to ITO can be converted into a strongly bonded form, thereby curtailing the migration of MeO-2PACz on the ITO surface during the spin-coating process, as well as inhibiting shedding that may occur due to solvent washing during the device preparation process. SACS SAMs heighten the charge collection ability of SAMs and suppress interfacial recombination, as well as enhance the growth of the upper perovskite layer. Finally, the SACS-based SAMs device with a power conversion efficiency of 26.37%. The unencapsulated device based on SACS SAMs can be stored for at least 5000 h with little degradation in performance.
研究领域:
材料科学
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能源技术
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界面化学
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产品关联
DOI
PubMed
高影响因子
Nano Energy
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2020
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IF 16.602
Jinwen Hu,Danyang Wu,Chao Zhu,Ce Hao,Cuncun Xin,Jiangwei Zhang,Jingya Guo,Nannan Li,Guifeng Zhang,Yantao Shi
Emerging heterogeneous catalysts with metal atomically dispersed on supports (tentatively termed single-atom catalysts, SACs) exhibit many appealing features in a wide variety of catalytic reactions , such as high activity and nearly 100% atom utilization. However, the synthesis of SACs currently requires not only multiple procedures but also appropriate precursors with special structures. Herein, the molten-salt assistance is presented as an effective means that enables the use of common metal oxides (such as Fe 2 O 3 and Co 2 O 3 ) and small organic molecules as precursors for the preparation of carbon-supported SACs through one-pot pyrolysis . Molten salts as templates that can be easily removed after synthesis also contribute to the formation of porous and nitrogen-doped carbon with a high specific area. More importantly, benefiting from the strong polarizing force of molten salts, the ionic bonds in oxides can be destabilized at high temperature. Subsequently, metal ions released from solid oxides are transformed into atomically dispersed active sites after being trapped by nitrogen (N) atoms on the carbon support. The as-prepared SAC with atomically dispersed Fe–N 4 sites demonstrates high activity, outstanding stability and good methanol tolerance in the oxygen reduction reaction (ORR) in both alkaline and acidic media.
研究领域:
催化
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材料科学
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化学工程
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DOI
高影响因子
Carbon Energy
·
2023
·Vol. 5
·期 7
·e294
·
IF 20.5
Ruisong Li,Daoxiong Wu,Peng Rao,Peilin Deng,Jing Li,Junming Luo,Wei Huang,Qi Chen,Zhenye Kang,Yijun Shen,Xinlong Tian
As a carbon-free energy carrier, hydrogen has become the pivot for future clean energy, while efficient hydrogen production and combustion still require precious metal-based catalysts. Single-atom catalysts (SACs) with high atomic utilization open up a desirable perspective for the scale applications of precious metals, but the general and facile preparation of various precious metal-based SACs remains challenging. Herein, a general movable printing method has been developed to synthesize various precious metal-based SACs, such as Pd, Pt, Rh, Ir, and Ru, and the features of highly dispersed single atoms with nitrogen coordination have been identified by comprehensive characterizations. More importantly, the synthesized Pt- and Ru-based SACs exhibit much higher activities than their corresponding nanoparticle counterparts for hydrogen oxidation reaction and hydrogen evolution reaction (HER). In addition, the Pd-based SAC delivers an excellent activity for photocatalytic hydrogen evolution. Especially for the superior mass activity of Ru-based SACs toward HER, density functional theory calculations confirmed that the adsorption of the hydrogen atom has a significant effect on the spin state and electronic structure of the catalysts.
研究领域:
催化
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材料科学
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能源科学
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化学工程
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产品关联
DOI
高影响因子
JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
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2022
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IF 5.895
Yajing Fang,Weiwei Cao,Mengmeng Xia,Siyi Pan,Xiaoyun Xu
This study aims to evaluate the interaction of flavonoid–flavonoid by inhibiting the function of P-glycoprotein (P-gp). The cellular uptake of seven substrates and eleven co-incubated inhibitors was measured in KB/MDR cells. The effect of galangin or morin on the absorption of silibinin or wogonin was carried out in the rat everted gut sacs. Docking was performed to evaluate the interactions between inhibitors and P-gp. Most substrates were greatly enhanced by at least five co-incubated inhibitors. Conversely, the increased uptake of substrates coincided with a decrease or without affecting the uptake of inhibitors, implying a competitive/non-competitive inhibition on P-gp. The enhancement effect by galangin or morin on the transport of silibinin or wogonin was verified in everted gut sacs. Docking explained the inhibition of flavonoids on P-gp by competitively binding to the ATP site. These results provide a strategy for increasing the absorption of flavonoids by co-administration.
研究领域:
药理学
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细胞生物学
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分子生物学
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DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
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IF 15.1
Jingjing Li,Wei Xia,Yanna Guo,Ruijuan Qi,Xingtao Xu,Dong Jiang,Tao Wang,Yoshiyuki Sugahara,Jianping He,Yusuke Yamauchi
Iron-based single-atom catalysts (Fe-SACs) containing Fe–N 4 active sites have shown immense potential in the oxygen reduction reaction (ORR). However, the limited ability to adsorb O 2 and catalyze subsequent O–O bond breaking on Fe–N 4 sites has hindered their full potential, especially in acidic electrolytes. Here, we present an approach by utilizing a tunable curved surface to enhance the activity of Fe–N 4 active sites, with theoretical calculations, demonstrating that Fe–N 4 sites anchored on low–curvature surfaces (lc-Fe-N 4 ) is favirable for ORR. Experimental results show that the catalyst exhibits excellent catalytic activity and stability for ORR in acidic electrolytes, with a half-wave potential of 0.82 V vs. RHE, approaching that of commercial Pt/C. This work develops an approach for promoting the catalytic activity by anchoring atomically dispersed Fe–N 4 sites, unlocking their potential for extended use in electrocatalytic and energy storage applications.
研究领域:
材料科学
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电化学
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催化
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能源存储
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产品关联
DOI
高影响因子
Nature Communications
·
2023
·Vol. 14
·期 1
·1-15
·
IF 16.6
Lu Xiangyu,Kuai Le,Huang Fang,Jiang Jingsi,Song Jiankun,Liu Yiqiong,Chen Si,Mao Lijie,Peng Wei,Luo Ying,Li Yongyong,Dong Haiqing,Li Bin,Shi Jianlin
Psoriasis is a common inflammatory disease of especially high recurrence rate (90%) which is suffered by approximately 3% of the world population. The overexpression of reactive oxygen species (ROS) plays a critical role in psoriasis progress. Here we show that biomimetic iron single-atom catalysts (FeN 4 O 2 -SACs) with broad-spectrum ROS scavenging capability can be used for psoriasis treatment and relapse prevention via related gene restoration. FeN 4 O 2 -SACs demonstrate attractive multiple enzyme-mimicking activities based on atomically dispersed Fe active structures, which are analogous to those of natural antioxidant enzymes, iron superoxide dismutase, human erythrocyte catalase, and ascorbate peroxidase. Further, in vitro and in vivo experiments show that FeN 4 O 2 -SACs can effectively ameliorate psoriasis-like symptoms and prevent the relapse with augmented efficacy compared with the clinical drug calcipotriol. Mechanistically, estrogen receptor 1 (ESR1) is identified as the core protein upregulated in psoriasis treatment through RNA sequencing and bioinformatic analysis. Together, this study provides a proof of concept of psoriasis catalytic therapy (PCT) and multienzyme-inspired bionics (MIB).
研究领域:
药学
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材料科学
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生物医学工程
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皮肤科
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产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）