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ANALYTICAL CHEMISTRY · 2019 · IF 6.35

Fe–N–C Single-Atom Nanozymes for the Intracellular Hydrogen Peroxide Detection

Lei Jiao,Weiqing Xu,Hongye Yan,Yu Wu,Chunrong Liu,Dan Du,Yuehe Lin,Chengzhou Zhu

Recently, in situ detection of hydrogen peroxide (H2O2) generated from live cells have caused tremendous attention, because it is of great significance in the control of multiple biological processes. Herein, Fe–N–C single-atom nanozymes (Fe–N–C SAzymes) with intrinsic peroxidase-like activity were successfully prepared via high-temperature calcination using FeCl2, glucose, and dicyandiamide as precursors. The Fe–N–C SAzymes with FeNx as active sites were similar to natural metalloproteases, which can specifically enhance the peroxidase-like activity rather than oxidase-like activity. Accordingly, owing to the excellent catalytic efficiency of the Fe–N–C SAzymes, colorimetric biosensing of H2O2 in vitro was performed via a typical 3,3′,5,5′-tetramethylbenzidine induced an allochroic reaction, demonstrating the satisfactory specificity and sensitivity. With regard to the practical application, in situ detection of H2O2 generated from the Hela cells by the Fe–N–C SAzymes was also performed, which can expand the applications of the newborn SAzymes.

研究领域: 生物化学 · 纳米医学 · 分析化学
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Nature Communications · 2025 ·Vol. 16 ·期 1 ·1-17 · IF 15.7

NIR-triggering cobalt single-atom enzyme switches off-to-on for boosting the interactive dynamic effects of multimodal phototherapy

Dai Hao,Han Ali,Wang Xijun,Zhu Peng,Wang Dingsheng,Wang Yuguang

Noninvasive phototherapy with functional preservation is considered to be a promising cancer therapeutic method. However, the clinical application of tumor phototherapy is severely restrained by the lack of appropriate multimodal phototherapy agents exhibiting an ideal tissue penetration depth to maximize the antitumor efficiency as well as to maintain important tissue functions. Herein, an innovative near-infrared ray (NIR)-triggered photodynamic-photocatalytic-photothermal therapy (PDT-PCT-PTT) agent based on an atomically dispersed cobalt single-atom enzyme (Co-SAE) anchored on hollow N-doped carbon sphere (HNCS) has been strategically developed. Reactive oxygen species (ROS) are highly activated and amplified through both the photogenerated electrons and the photothermal conversion induced by NIR irradiation, as systematically demonstrated by the experimental and density functional theory (DFT) calculation results. Mild hyperthermia is eventually achieved through apoptosis and ferroptosis caused by ROS, significantly boosting the interaction of ROS dynamic effects and thermodynamic effects in the tumor microenvironment (TME). More importantly, Co-SAEs/HNCS not only causes multimodal damage through limited TME products but also preserves important organ functions by the induction of mild local hyperthermia. This work expands the biomedical application field of SAEs and presents an innovative all-in-one, multimodal concept for the noninvasive treatment of head and neck cancer.

CAS / MDL: 95-54-5 54827-17-7
研究领域: 生物医学工程 · 癌症治疗 · 纳米医学
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY · 2024 · IF 4.3

Smartphone-based colorimetric paper chip sensor using single-atom nanozyme for the detection of carbofuran pesticide residues in vegetables

Lifan Zhang,Ziyue Lang,Bozhi Lu,Tinglan Yang,Xinyi Zhang,Muxue Wang,Xiaomei Zhang,Hongmei Cao,Daixin Ye

Carbofuran (CBF), which exhibit high toxicity, persistent residues, ease of accumulation, and resistance to degradation, pose serious threats to human health and harm the ecological environment. Therefore, there is an urgent need to develop a rapid and accurate method for detecting CBF. In this work, a low-cost, portable, and easy-to-use paper chip biosensor was developed, integrating smartphones for the detection of CBF pesticide residues. This biosensor facilitates rapid on-site testing, meeting the needs for immediate analysis. CBF has the ability to inhibit acetylcholinesterase (AChE) activity. In the presence of AChE, acetylthiocholine (ATCh) is hydrolyzed to produce thiocholine (TCh). TCh, in turn, can inhibit the catalytic activity of Ni-N-C single-atom nanozymes (SAzyme) synthesized using Ni(OH) 2 nanochip as a metal precursor, which possess high peroxidase activity. Consequently, the concentration of CBF can be determined by observing the resultant color changes. The results showed that this sensor had a good linear response in the range of CBF concentration from 10 to 500 ng/mL, and the LOD was as low as 8.79 ng/mL. In testing three actual samples—Chinese cabbage, cabbage, and lettuce—the recoveries ranged from 81.09% to 125.27%. This demonstrated that the proposed smartphone-based colorimetric paper chip sensor, utilizing Ni-N-C SAzyme, offers an immediate, convenient, and rapid new strategy for detecting CBF.

研究领域: 环境科学 · 分析化学 · 生物传感器 · 食品安全 · 农药检测
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ACS Applied Materials & Interfaces · 2020 · IF 8.758

Single-Atom Enzyme-Functionalized Solution-Gated Graphene Transistor for Real-Time Detection of Mercury Ion

Lili Yao,Shengjie Gao,Shuai Liu,Yulong Bi,Rongrong Wang,Hao Qu,Yuen Wu,Yu Mao,Lei Zheng

Mercury ion (Hg2+), a bioaccumulating and toxic heavy metal, can cause severe damages to the environment and human health. Therefore, development of high-performance Hg2+ sensors is highly desirable. Herein, we construct a uniform dodecahedral shaped N-doped carbon decorated by single Fe site enzyme (Fe-N-C SAE), which exhibits good performance for Hg2+ detection. The N atom on Fe-N-C SAE can specifically recognize Hg2+ through chelation between Hg2+ and N atom, while the catalytic site on the single-atom enzyme acts as a signal amplifier. The Fe-N-C SAE-functionalized solution-gated graphene transistor exhibits a dramatic improvement in the selectivity and sensitivity of the devices. The sensor can rapidly detect Hg2+ down to 1 nM within 2 s. Besides, a relatively good repeatability and reproducibility for the detection of Hg2+ have also been found in our sensor platform. Our findings expand the application of single-atom catalysts in the field of food safety and environmental monitoring.

研究领域: 环境科学 · 材料科学 · 分析化学 · 纳米技术 · 传感器技术
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Advanced Healthcare Materials · 2024 · IF 10

Atomically Engineered Chlorine Coordination of Iron in Active Centers for Selectively Catalytic H2O2 Decomposition Toward Efficient Antitumor-Specific Therapy

Wei Li,Daomei Chen,Chungang Min,Xiaoqian Ma,Xikun Yang,Jiaqiang Wang

The intervention of endogenous H 2 O 2 via nanozymes provides a potential antitumor-specific therapy; however, the role of the nanozyme structure in relation to the selective decomposition of H 2 O 2 to hydroxyl radicals (•OH) is yet to be fully understood, which limits the development of this therapeutic approaches. Herein, an iron single-atom nanozyme (Fe─N 2 Cl 2 ─C SAzyme) is reported, which is prepared through precise Fe─Cl coordination based on the construction of a characteristic Fe-containing molecule. Fe─N 2 Cl 2 ─C exhibits efficient catalytic H 2 O 2 decomposition (2.19 × 10 6 m m −1 s −1 ), which is the highest among reported SAzymes. More importantly, it is found that H 2 O 2 selectively decomposed into •OH on the Fe─N 2 Cl 2 ─C surface, which is attributable to the d orbitals of the Fe active center matching the O-2 p electrons of the adsorbed hydroxide (*OH) intermediate. Fe─N 2 Cl 2 ─C is strongly cytotoxic toward a variety of cancer-cell lines in vitro but not to normal cells. Furthermore, Fe─N 2 Cl 2 ─C shows an outstanding specific therapeutic effect in vivo; it efficiently destroys solid malignant tumors without injuring normal tissue. Altogether, these findings highlight the selective catalytic decomposition of H 2 O 2 to •OH, which is achieved by engineering the active center on the atomic level, thereby providing an avenue for the development of specific nanomedicines with efficient antitumor activities.

研究领域: 材料科学 · 纳米技术 · 生物医学工程 · 癌症研究 · 化学生物学
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