FOOD CHEMISTRY
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2025
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IF 9.8
Shu Yang,Yijun Ren,Ganbing Zhang,Hui Xu
Single-atom nanozymes (SAzymes) exhibit superior catalytic activity, making it a promising candidate for constructing biosensors. Herein, we constructed a hollow carbon nanocages supported, N and O double-coordinated Fe SAzymes (HCNs@Fe SAs) through a template and pyrolysis strategy. Abundant oxygen atoms in pre-modified template SiO 2 @resorcinol-formaldehyde provided enough binding sites and promoted the dispersion and stabilization of metal atoms. Compared with non-O modified nanozymes, HCNs@Fe SAs exhibited an 8-fold enhancement in catalytic efficiency. Benefiting from its exceptional peroxide-like activity, a straightforward and dependable colorimetric sensing platform was developed to assess the activity of Acetylcholinesterase and its inhibitor organophosphorus pesticide (OP) in real water samples and fruit substrates, with the limit of detection of 0.02318 mU mL −1 and 0.85 ng mL −1 , respectively. An OPs test paper was also designed for point-of-care determination of OP with satisfactory sensitivity. This study provides a new strategy of template pre-modification to design SAzymes with enhanced catalytic efficiency.
研究领域:
生物传感
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催化材料
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环境检测
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Energy Chemistry
·
2024
·
IF 14
Wenkang Miao,Ronghui Hao,Lu Gan,Wanyin Xu,Zihan Wang,Wenxin Lin,Heguang Liu,Yinchun Lyu,Qianqian Li,Jinyang Xi,Anmin Nie,Jinsong Wu,Hongtao Wang
Platinum-based (Pt) catalysts are notoriously susceptible to deactivation in industrial chemical processes due to carbon monoxide (CO) poisoning. Overcoming this poisoning deactivation of Pt-based catalysts while enhancing their catalytic activity, selectivity, and durability remains a major challenge. Herein, we propose a strategy to enhance the CO tolerance of Pt clusters (Pt n ) by introducing neighboring functionalized guest single atoms (such as Fe, Co, Ni, Cu, Sb, and Bi). Among them, antimony (Sb) single atoms (SAs) exhibit significant performance enhancement, achieving 99% CO selectivity and 33.6% CO 2 conversion at 450 °C. Experimental results and density functional theory (DFT) calculations indicate the optimization arises from the electronic interaction between neighboring functionalized Sb SAs and Pt clusters, leading to optimal 5 d electron redistribution in Pt clusters compared to other functionalized guest single atoms. The redistribution of 5 d electrons weaken both the σ donation and π backdonation interactions, resulting in a weakened bond strength with CO and enhancing catalyst activity and selectivity. In situ environmental transmission electron microscopy (ETEM) further demonstrates the exception thermal stability of the catalyst, even under H 2 at 700 °C. Notably, the functionalized Sb SAs also improve CO tolerance in various heterogenous catalysts, including Co/CeO 2 , Ni/CeO 2 , Pt/Al 2 O 3 , and Pt/CeO 2 -C. This finding provides an effective approach to overcome the primary challenge of CO poisoning in Pt-based catalysts, making their broader applications in various industrial catalysts.
研究领域:
材料科学
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催化化学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
ANALYTICAL CHEMISTRY
·
2019
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IF 6.35
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
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纳米医学
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分析化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Nature Communications
·
2022
·Vol. 13
·期 1
·1-10
·
IF 17.694
Zhang Zhirong,Feng Chen,Wang Dongdi,Zhou Shiming,Wang Ruyang,Hu Sunpei,Li Hongliang,Zuo Ming,Kong Yuan,Bao Jun,Zeng Jie
The homogeneity of single-atom catalysts is only to the first-order approximation when all isolated metal centers interact identically with the support. Since the realistic support with various topologies or defects offers diverse coordination environments, realizing real homogeneity requires precise control over the anchoring sites. In this work, we selectively anchor Ir single atoms onto the three-fold hollow sites (Ir 1 /T O –CoOOH) and oxygen vacancies (Ir 1 /V O –CoOOH) on defective CoOOH surface to investigate how the anchoring sites modulate catalytic performance. The oxygen evolution activities of Ir 1 /T O –CoOOH and Ir 1 /V O –CoOOH are improved relative to CoOOH through different mechanisms. For Ir 1 /T O –CoOOH, the strong electronic interaction between single-atom Ir and the support modifies the electronic structure of the active center for stronger electronic affinity to intermediates. For Ir 1 /V O –CoOOH, a hydrogen bonding is formed between the coordinated oxygen of single-atom Ir center and the oxygenated intermediates, which stabilizes the intermediates and lowers the energy barrier of the rate-determining step.
研究领域:
催化
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材料科学
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电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACTA PHYSICO-CHIMICA SINICA
·
2025
·
IF 13.5
Yuchen Zhou,Huanmin Liu,Hongxing Li,Xinyu Song,Yonghua Tang,Peng Zhou
The intrinsic surface atomic configuration of photocatalyst without unstable or difficult-to-generate atomic vacancies often limits the formation of effective interaction between metal single atom (MSA) cocatalyst and photocatalyst, thus inhibiting the stability and performance improvement of single-atom photocatalysts. In this study, we present a convenient and cost-effective photochemical oxygen reduction reaction (ORR) mechanism to prepare thermodynamically stable noble metal single-atom cocatalysts on TiO 2 photocatalyst under mild condition (only consuming water and oxygen at 101,325 Pa and 25 °C). The first-principles simulation firstly theoretically reveals that the intrinsic surface configuration of TiO 2 can only produce unstable Pt―O 2 structure. However, ORR occurring on TiO 2 can not only provide one foreign oxygen to coordinate with Pt single atom (PtSA), but also induce one surface lattice oxygen to move toward PtSA, promoting the formation of one thermodynamically stable Pt―O 4 species, demonstrated by the experimental synthesis of PtSA on TiO 2 in oxygen atmosphere instead of inert atmosphere. The obtained stable PtSA-TiO 2 photocatalysts exhibit a photocatalytic rate of 320.4 mmol·g −1 ·h −1 for the coproduction of high-purity hydrogen and value-added acetaldehyde with a selectivity of 99.65%, three-fold higher than the activity of Pt nanoparticles-loaded TiO 2 . This strategy is further extended to other noble metals, such as Rh and Pd.
研究领域:
化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Zhou Yang,Meng Xiang,Yunfeng Zhu,Jia Hui,Yong Jiang,Shuang Dong,Chengbin Yu,Junfei Ou,Hengfei Qin
Pt/C is a practical electrocatalyst for oxygen reduction reaction (ORR) in metal-air batteries and fuel cells, however, also suffers the drawbacks of high cost and instability, which have propelled people to search for new substitutes, such as single-atom metal electrocatalysts. Herein, C 4 N was firstly synthesized from 2,3-diyldiamine phenazine via one-step hydrothermal method rather than the traditional way that two monomers react in organic solvent, and then loaded with single-atom metal (Pt or Ru) to form new electrocatalysts. The so-formed M@C 4 N (M = Pt or Ru) electrocatalysts show more excellent ORR performances with higher half-wave potential and better stability and methanol tolerance as compared with the commercial Pt/C. Specifically, the half-wave potential of 1%Pt@C 4 N and 0.5%Ru@C 4 N is 0.861 V and 0.828 V, respectively. Density functional theory calculations reveal that 1%Pt@C 4 N has stronger adsorption of reactant species and faster kinetics than 0.5%Ru@C 4 N in ORR pathway.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Ting Wang,Fuli Sun,Shoujie Liu,Guilin Zhuang,Benxia Li
Supported Cu single-atom (Cu-SA) catalysts have exhibited unique activity and selectivity in CO 2 reduction, but they generally suffer from the easy transformation of active Cu δ+ into inactive Cu 0 . Herein, porous TiO 2 supported Cu single atoms (Cu-SAs/TiO 2 ) photocatalyst was fabricated and dioxygen (O 2 ) enhanced photocatalytic CO 2 reduction performance of Cu-SAs/TiO 2 was investigated by in-situ characterizations and theoretical calculations. The results showed that both activity and stability of Cu-SAs/TiO 2 photocatalyst could be improved by feeding a small amount of O 2 (117.6 ppm) in the reaction system. The competitive electron transfer to O 2 on Cu-SAs/TiO 2 maintained dynamic stability of Cu δ+ active sites, and O 2 -derived *OOH species lowered the formation energy barrier of key intermediate *COOH as well as delivered *H species for accelerating intermediates protonation process. Total yield rate of CH 4 and CO reached 34.64 μmol·g cat ·h −1 for CO 2 photoreduction over Cu-SAs/TiO 2 after introducing 117.6 ppm O 2 , accompanied by enhanced durability.
研究领域:
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
ANALYTICA CHIMICA ACTA
·
2024
·
IF 5.7
Mengqiong Zhang,Guowen Wang,Jiping Chen,Xianbo Lu
Bisphenol compounds (BPA, BPS, BPAF, etc.) are one class of the most important and widespread pollutants that poses severe threat to human health and the ecological environment. Because of the presence of multiple bisphenols in environmental and food samples, it is urgent and challenging to develop a rapid and cheap technique for simultaneously detecting BPA and its analogues. In this study, a series of M - N -C (M = Cu, Mg, Ni, Co, Fe, K) single-atom nanozymes (SAzymes) were created by simulating the structure of natural enzyme molecules, which were used as novel sensing platform for the fabrication of electrochemical sensors. Through systematic screening and characterization, it was interestingly discovered that the electrochemical sensor based on Cu- N -C SAzymes exhibited the best sensing performance for bisphenols among all SAzymes, which catalyzed not only BPA like tyrosinase, but also showed excellent catalytic capacity beyond tyrosinase (tyrosinase has no catalytic activity for BPS, BPAF, etc.), and achieved potential-resolved simultaneous rapid detection of BPA, BPS and BPAF. Further structure-activity relationship and catalytic mechanism characterizations of Cu- N -C SAzymes revealed that the presence of single atom Cu was predominantly in the form of Cu + and Cu 2+ , which were anchored onto graphene nanosheet support through four coordination bonds with pyridinic N and pyrrolic N and acted as highly efficient active centers for electrocatalytic oxidation of bisphenols. The developed electrochemical sensing method exhibited excellent selectivity, sensitivity, and reliability for the rapid detection of multiple bisphenols in actual samples.
研究领域:
分析化学
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环境科学
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材料科学
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纳米技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Yuhui Huang,Ruyu Xie,Kaitao Li,Rui Tian,Yanjun Lin,Chao Lu
Currently, much attention has been paid to the efforts to stabilize and regulate single atoms through supports to obtain decent electrocatalytic behaviors. However, little concern was given to the effect of single atoms on modulating the electronic structure of supports, despite the catalytic activities and large quantities of supports in the catalytic reactions. Herein, we have localized Ru single atoms onto two-dimensional layered double hydroxide (NiFe-LDH) and studied the role of Ru single atoms in adjusting the electronic structure of the NiFe-LDH support. Spin polarization of 3d electrons for Fe and electron redistribution in NiFe-LDH were effectively modulated through the interaction between Ru single atoms and NiFe-LDH. As a result, the luminol redox reaction and reactive oxygen revolution were simultaneously promoted by Ru single-atom-modulated NiFe-LDH, manifested as boosted electrochemiluminescence (ECL). Therefore, we have provided valid information to reveal the regulation effect of single atoms on the spin state and electronic structure of the supports. It is anticipated that our strategy may arouse wide interest in manipulating single-atom-modulated supports.
研究领域:
材料科学
·
电化学
·
催化
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Catalysis
·
2022
·
IF 13.7
Danfeng Wu,Sixu Liu,Mingqi Zhong,Jiafei Zhao,Congcong Du,Yanling Yang,Yifei Sun,Jingdong Lin,Shaolong Wan,Shuai Wang,Jianyu Huang,Yali Yao,Zhe Li,Haifeng Xiong
Metal single-atom catalysts (SACs) have attracted extensive interest because of their maximum atom efficiency and potentially good performances. However, the understanding of the catalytic behavior and the stability of SACs in high-temperature catalytic reactions remains a major challenge, especially under reducing conditions. In this work, we investigated the nature and stability of Rh/CeO2 SACs with different Rh loadings (0.2–4 wt % Rh) during syngas conversion (260 °C, 2 MPa). Using CO-DRIFTS, we found that atomically dispersed Rh was dispersed on Rh/CeO2 catalysts with an Rh loading up to 3 wt %. The Rh/CeO2 catalysts were stable in H2 up to 350 °C, while Rh nanoclusters were formed in CO at 200 °C. During syngas conversion at 260 °C, the Rh single atoms (Rhiso) on a 0.5 wt % Rh/CeO2 SAC slowly agglomerated to form Rh nanoclusters (RhNC) and a Rhiso/RhNC ratio of ∼1:2.5 was obtained after ∼10 h time-on-stream run. Furthermore, the Rhiso/RhNC ratio did not change with further reaction, indicating that the reaction reached steady state after a 10 h run. After the catalysts reached steady state (∼10 h), the Rhiso/RhNC ratio on the spent Rh/CeO2 catalysts decreased with the increase in Rh loadings, while the reactivity increased first and then decreased. We observed an optimal value of Rhiso/RhNC ≈ 1:3 on the 1 wt % Rh/CeO2 catalyst, showing the maximum reaction rates of CO (rCO) and ethanol selectivity (SEtOH) of 85.8 μmol/s/gRh and 26.2%, respectively. This indicated that the combination of Rh single atoms and Rh nanoclusters is beneficial to the ethanol selectivity and reaction rate, which was confirmed by DFT simulations. Moreover, the ratios of Rhiso/RhNC on the spent catalysts under the steady state have good relationships with the CO conversion rate and product selectivity in the reaction.
研究领域:
催化化学
·
材料科学
✓ 已验证
DOI
高影响因子
Nature Communications
·
2022
·Vol. 13
·期 1
·1-10
·
IF 17.694
Shi Xiaowei,Dai Chao,Wang Xin,Hu Jiayue,Zhang Junying,Zheng Lingxia,Mao Liang,Zheng Huajun,Zhu Mingshan
Single-site cocatalysts engineered on supports offer a cost-efficient pathway to utilize precious metals, yet improving the performance further with minimal catalyst loading is still highly desirable. Here we have conducted a photochemical reaction to stabilize ultralow Pt co-catalysts (0.26 wt%) onto the basal plane of hexagonal ZnIn 2 S 4 nanosheets (Pt SS -ZIS) to form a Pt-S 3 protrusion tetrahedron coordination structure. Compared with the traditional defect-trapped Pt single-site counterparts, the protruding Pt single-sites on h -ZIS photocatalyst enhance the H 2 evolution yield rate by a factor of 2.2, which could reach 17.5 mmol g −1 h −1 under visible light irradiation. Importantly, through simple drop-casting, a thin Pt SS -ZIS film is prepared, and large amount of observable H 2 bubbles are generated, providing great potential for practical solar-light-driven H 2 production. The protruding single Pt atoms in Pt SS -ZIS could inhibit the recombination of electron-hole pairs and cause a tip effect to optimize the adsorption/desorption behavior of H through effective proton mass transfer, which synergistically promote reaction thermodynamics and kinetics.
研究领域:
材料科学
·
能源化学
·
环境科学
✓ 已验证
DOI
高影响因子
iScience
·
2024
·
IF 4.6
Ai-Ping Yan,Yu-Jue Qiu,Xing-En Wang,Guang-Hua Wang,Xian-Kui Wei,Xin-Tian Li,Xiao-Die Chen,Xing Shang,Shun-Liu Deng,Jian-Wei Zheng,Su-Yuan Xie
C 3 N 4 is widely applied in the synthesis of single-atom catalysts. However, understanding on the active site and the reaction mechanism is not fully in consensus. Especially, bare studies have considered the coordination environment of the single-atomic dopant and the effect of nitrogen vacancy on C 3 N 4 . In this study, we found that the presence of nitrogen vacancies promotes the activation of water and reduces the activation energy barrier for hydrogen generation. The results show that a synergistic effect between single-atom Pt and nitrogen vacancies enables the catalyst to achieve a superior hydrogen production rate of 3,890 μmol/g/h, which is 16.8 times higher than that of pristine C 3 N 4 . Moreover, the catalyst is also applicable for photocatalytic hydrogen production from seawater without significantly decreased hydrogen production rate. This study paves the way for the rational design and optimization of next-generation photocatalysts for sustainable energy applications, particularly in solar-driven hydrogen production.
研究领域:
材料科学
·
能源化学
✓ 已验证
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）