ENERGY & FUELS
·
2023
·
IF 5.3
Jun Tang,Jinzhao Huang,Sixuan Zhang,Zehui Liu,Xiaolong Deng
Metal-phase MoS2 (1T-MoS2) is considered a promising candidate as a catalyst for the hydrogen evolution reaction (HER). However, the instability of 1T-MoS2 limits its electrocatalytic activity. Herein, we first synthesized 1T-MoS2 with excellent HER catalytic performance by a simple one-pot hydrothermal strategy of introducing the d-electron-rich transition metal atom Ni into MoS2. A bimetallic monatomic catalyst (Pt@1T-MoS2–Ni) was also prepared by modifying 1T-MoS2–Ni with Pt single atoms (Pt SAs). Experiments show that the electron transfer caused by Ni doping leads to the 1T phase transition, and the modification of Pt SAs further improves the electrical conductivity. These two factors synergistically modulate the electronic composition of MoS2 and increase the number of reactive sites. In consequence, the Pt@1T-MoS2–Ni catalyst exhibits significantly enhanced HER activity, achieving an overpotential as low as 76 mV at 10 mA/cm2 with the corresponding Tafel slope of only 46 mV/dec. Moreover, the current attenuation is negligible within 12 h, surpassing the performance of MoS2. This study offers ideas for improving the efficiency and stability of 1T-MoS2 catalyst designs.
研究领域:
材料科学
·
电催化
·
能源化学
✓ 已验证
产品关联
DOI
高影响因子
CARBON
·
2023
·
IF 10.9
Tiantian Ma,Peng Wang,Hua-Jie Niu,Zhongxuan Che,Guozheng Li,Wei Zhou
Exposing more catalytic active sites is an effective strategy to enhance the catalyst activity for hydrogen evolution reaction (HER). Herein, Ti 3 C 2 T x MXene served as a substrate to load thin and curved 2 H –MoSe 2 nanosheets by a typical hydrothermal method , forming MoSe 2 /MXene heterointerface with the fully exposed Mo edge sites. And then, atomically dispersed Ru single atoms (RuSAs) were successfully anchored on the MoSe 2 /MXene (RuSAs@MoSe 2 -MXene). The X-ray absorption near edge structure (XANES) demonstrates that Ru is loaded as single atoms on MoSe 2 and MXene . The prepared sample exhibits improved catalytic activity with a small overpotential of 49 mV at 10 mA cm −2 and a low Tafel slope of 52 mV dec −1 for HER in 0.5 M H 2 SO 4 . It also exhibits excellent stability with a small attenuation voltage of 10 mV for 120 h at 10 mA cm −2 in 0.5 M H 2 SO 4 . When assembled into a two-electrode system of RuSAs@MoSe 2 -MXene||RuO 2 , it only requires a relatively low potential of 1.626 V at 10 mA cm −2 to drive overall water splitting (OWS). Control experiments disclose the highly improved performance can be primarily attributed to the introduced RuSAs and MoSe 2 /MXene heterointerfaces exposing more active sites of Ru and Mo. Moreover, the high conductivity of MXene can increase charge transfer in HER process. The interface engineering with multiple interfaces can provide fresh impetus for the development of efficient HER catalysts.
研究领域:
材料科学
·
催化化学
·
能源化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Catalysis
·
2023
·
IF 12.9
Xu Yu,Han Tian,Zhengqian Fu,Fenglai Pei,Lingxin Peng,Ge Meng,Fantao Kong,Yafeng Chen,Chang Chen,Ziwei Chang,Xiangzhi Cui,Jianlin Shi
The hydrogen spillover effect on metal-supported electrocatalysts is of great significance in hydrogen-involved reactions, especially in a hydrogen oxidation reaction (HOR). Herein, a facile thermal reduction method has been adopted to synthesize W18O49 (WO2.72) nanospheres decorated with single nickel atoms, and the obtained Ni-WO2.72-T (1.20 wt % Ni) was used as a probe catalyst for investigating the hydrogen spillover effect, which exhibits enhanced HOR performance, stability, and resistance to CO poisoning in acidic electrolytes. Based on in situ Raman spectroscopy and the density functional theory (DFT) calculation, a synergistic effect between Ni single-atom active sites and the hydrogen spillover effect is proposed to contribute to the HOR performance on Ni-WO2.72-T. Briefly, the introduction of single Ni atoms induces electron redistribution on Ni-WO2.72-T, making Ni atoms positively charged for H2 adsorption and activation, and on the other hand, the reversible phase transformation between WO2.72 and HxWO2.72 facilitates H* transfer from Ni to WO2.72, i.e., hydrogen spillover, resulting in elevating the HOR catalytic activity. Both experimentation and theoretical calculations demonstrate that the reversible phase transformation of the WO2.72 substrate strengthens the hydrogen spillover effect and thus elevates the HOR catalytic performance, which is believed to be helpful in designing highly active catalysts for hydrogen-involving reactions.
研究领域:
电化学
·
催化材料
·
理论计算
✓ 已验证
产品关联
DOI
高影响因子
SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
·
2024
·
IF 4.3
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
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ANALYTICAL CHEMISTRY
·
2025
·
IF 6.7
Jingyuan Guo,Guo Wang,Yunfan She,Kai Li,Yujia Liu,Zhiyi Sun,Zhengbo Chen
Single-atom nanozymes have made important progress in the field of sensors, but their catalytic performance as natural enzyme substitutes is far from satisfactory. We describe here a FeFe dual single-atom nanozyme (Fe2N6/CN) with a Fe loading of 0.89 wt %, and it shows a synergistic effect and a peroxidase (POD)-like activity. Especially, the Fe2N6/CN nanozyme shows an excellent specific activity (315.4 U μmol–1). The values of catalytic rate constant (kcat) and catalytic efficiency (kcat/Km) for the Fe2N6/CN with 3,3′,5,5′-tetramethylbenzidine (TMB) are 23.8 s–1 and 8.24 × 104 M–1 s–1, respectively, and with H2O2, they are 30.8 s–1 and 0.919 × 103 M–1 s–1, respectively. Density functional theory calculations reveal that Fe2N6/CN possesses excellent POD-like activity. Based on the POD-like activity of Fe2N6/CN, we design a Fe2N6/CN nanozyme chemical tongue for the colorimetric recognition of aromatic amines using three wavelengths as array’s channels. The data interpretation using linear discriminant analysis, clustering heat map, etc., shows excellent clustering separation and classification of aromatic amines. Furthermore, this chemical tongue can simultaneously recognize mixtures of different molar ratios, quantitatively determine different concentrations of individual aromatic amines, and even identify unknown samples. This preparation strategy not only provides a promising pathway for the utilization of nanozymes but also highlights the potential of dual single atoms as an attractive platform for design of sensor arrays.
研究领域:
纳米酶
·
催化
·
传感器
·
化学传感
·
材料科学
·
分析化学
·
计算化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Nature Communications
·
2020
·Vol. 11
·期 1
·1-9
·
IF 12.121
Liu Kaipeng,Zhao Xintian,Ren Guoqing,Yang Tao,Ren Yujing,Lee Adam Fraser,Su Yang,Pan Xiaoli,Zhang Jingcai,Chen Zhiqiang,Yang Jingyi,Liu Xiaoyan,Zhou Tong,Xi Wei,Luo Jun,Zeng Chaobin,Matsumoto Hiroaki,Liu Wei,Jiang Qike,Wilson Karen,Wang Aiqin,Qiao Botao,Li Weizhen,Zhang Tao
Single-atom catalysts (SACs) have demonstrated superior catalytic performance in numerous heterogeneous reactions. However, producing thermally stable SACs, especially in a simple and scalable way, remains a formidable challenge. Here, we report the synthesis of Ru SACs from commercial RuO 2 powders by physical mixing of sub-micron RuO 2 aggregates with a MgAl 1.2 Fe 0.8 O 4 spinel. Atomically dispersed Ru is confirmed by aberration-corrected scanning transmission electron microscopy and X-ray absorption spectroscopy. Detailed studies reveal that the dispersion process does not arise from a gas atom trapping mechanism, but rather from anti-Ostwald ripening promoted by a strong covalent metal-support interaction. This synthetic strategy is simple and amenable to the large-scale manufacture of thermally stable SACs for industrial applications.
研究领域:
催化
·
材料科学
·
化学工程
✓ 已验证
DOI
PubMed
高影响因子
Nature Communications
·
2023
·Vol. 14
·期 1
·1-16
·
IF 16.6
Huang Biao,Tang Tao,Chen Shi-Hui,Li Hao,Sun Zhi-Jun,Zhang Zhi-Lin,Zhang Mingxi,Cui Ran
The blood-brain barrier breakdown, as a prominent feature after traumatic brain injury, always triggers a cascade of biochemical events like inflammatory response and free radical-mediated oxidative damage, leading to neurological dysfunction. The dynamic monitoring the status of blood-brain barrier will provide potent guidance for adopting appropriate clinical intervention. Here, we engineer a near-infrared-IIb Ag 2 Te quantum dot-based Mn single-atom catalyst for imaging-guided therapy of blood-brain barrier breakdown of mice after traumatic brain injury. The dynamic change of blood-brain barrier, including the transient cerebral hypoperfusion and cerebrovascular damage, could be resolved with high spatiotemporal resolution (150 ms and ~ 9.6 µm). Notably, the isolated single Mn atoms on the surface of Ag 2 Te exhibited excellent catalytic activity for scavenging reactive oxygen species to alleviate neuroinflammation in brains. The timely injection of Mn single-atom catalyst guided by imaging significantly promoted the reconstruction of blood-brain barrier and recovery of neurological function after traumatic brain injury.
研究领域:
神经科学
·
纳米技术
·
生物医学工程
·
诊疗学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2024
·
IF 10.8
Zhisong Liu,Haomiao Xu,Yurui Fan,Wenjun Huang,Feng Yu,Zan Qu,Naiqiang Yan
Ruthenium single-atom catalysts have great potential in ammonia-selective catalytic oxidation (NH3–SCO); however, the stable sp3 hybrid orbital of NH3 molecules makes N(sp3)–H dissociation a challenge for conventional symmetrical metallic oxide catalysts. Herein, we propose a heterogeneous interface reverse atom capture strategy to construct Ru with unique asymmetric Ru1N2O1 coordination. Ru1N2O1/CeO2 exhibits intrinsic low-temperature conversion (T100 at 160 °C) compared to symmetric coordinated Ru-based (280 °C), Ir-based (220 °C), and Pt-based (200 °C) catalysts, and the TOF is 65.4 times that of Ag-based catalysts. The experimental and theoretical studies show that there is a strong d–p orbital interaction between Ru and N atoms, which not only enhances the adsorption of ammonia at the Ru1N2O1 position but also optimizes the electronic configuration of Ru. Furthermore, the affinity of Ru1N2O1/CeO2 to water is significantly weaker than that of conventional catalysts (the binding energy of the Pd3Au1 catalyst is −1.19 eV, but it is −0.39 eV for our material), so it has excellent water resistance. Finally, the N(sp3)–H activation of NH3 requires the assistance of surface reactive oxygen species, but we found that asymmetric Ru1N2O1 can directly activate the N(sp3)–H bond without the involvement of surface reactive oxygen species. This study provides a novel principle for the rational design of the proximal coordination of active sites to achieve its optimal catalytic activity in single-atom catalysis.
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Huawang Zhao,Yuxin Xie,Bihong Lv,Guohua Jing,Yongdan Li
The CO 2 electrochemical reduction reactions (CO 2 ER) to produce high-value formate are crucial for closing the anthropogenic CO 2 cycle. Modulating the adsorption energy between *OCHO and Bi atoms in Bi-based catalysts could enhance both the activity and selectivity for formate formation. Here, a Bi/BiOBr nanosheet with highly dispersed Bi single atoms in intercalations was synthesized through NaBH 4 treatment of BiOBr, which retained the intercalated Bi atoms after electrolysis (Bi/BiOBr-D). The intercalated Bi atoms optimize the Bi-6p band center (0.016 eV) and charge distribution in Bi/BiOBr-D, enhancing the coupling between the O-2p orbitals of *OCHO and the Bi-6p orbitals as well as the electron transfer dynamics between Bi and the *OCHO intermediate, which improves the stability of the *OCHO intermediate during CO 2 ER. Further studies demonstrate that enhanced *OCHO adsorption reduces the Gibbs free energy barrier for the CO 2 →*OCHO process and suppressing the formation of the *H intermediate. Those advantages lead to high selectivity (FE of 96.83 %) in H-type cell, and excellent activity (j HCOO- of 815 mA/cm²) and productivity (15.22 mmol/h·cm²) in flow cell for formate production over Bi/BiOBr-D sample.
研究领域:
材料科学
·
电化学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Materials Chemistry A
·
2024
·Vol. 12
·期 26
·15966-15973
·
IF 10.7
Yan Wu,Qingqing Chen,Jiaping Liu,Kai Fang,Man Zhang,Tao Jing,Zhujie Li,Gang Wang
Precisely regulating the transfer path of charge carriers and triggering active sites is a robust yet extremely challenging strategy to realize efficient photocatalysis. Herein, we engineered a photocatalyst co-decorated with Pt single atoms (Pt1) and Pt nanoparticles (PtNP) to open up the transfer path of photo-generated electrons and holes, which allowed for the accurate fabrication and orientation of electron acceptor and donor active sites on different supports, such as La-doped SrTiO3 (La-STO), TiO2, g-C3N4 and MIL-125. In the case of La-STO, Pt1/PtNP/La-STO displayed roughly 16 and 26 times higher overall water-splitting activity than Pt1/La-STO and PtNP/La-STO. The experimental and theoretical analyses reveal that the enhancement of overall water-splitting performance occurs because of the co-decoration of electron acceptor (Pt1) and donor (PtNP) active sites on La-STO. Promisingly, this work demonstrates a novel method for accurately controlling active sites to obtain highly efficient photocatalysts.
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
·
2025
·
IF 7.7
Yunpeng Xing,Sihao Zhi,Liang Zhao,Hongda Zhang,Chengchao Yu,Teng Fei,Sen Liu,Haiyan Zhang,Tong Zhang
The graphene-based room-temperature chemiresistive gas sensors have low sensitivity (especially for ppb-level organophosphorous compounds, OPCs), limiting their practical applications. Herein, a novel coupling single-atom Cu and N-enriched, π-conjugated carbon nanodots (NCDs) strategy is proposed to synthesize graphene-based sensing materials with excellent room-temperature DMMP sensing performances. Taking rGO-NCDs-Cu as the example, the N-enriched structures facilitate the adsorption of DMMP by providing more active sites and strengthening the hydrogen bonding interactions between -NH 2 and DMMP molecules. The π-conjugated structures can construct large π-delocalization network promoting charge generation and transport. The N-enriched and π-conjugated structures also result in narrowing band gap of NCDs, effectively enabling the increase of carrier transfer rate. Moreover, the introduction of single-atom Cu sites with Cu-N 2 Cl 2 structure further strengthens the hydrogen bonding interactions between sensing materials and DMMP molecules. Benefiting from this novel coupling strategy, rGO-NCDs-Cu sensor shows high response value of 13.95 % towards 340 ppb DMMP at room temperature. Meanwhile, rGO-NCDs-Cu sensor exhibits short response time (77 s) and recovery time (198 s), low practical limit of detection (34 ppb), excellent repeatability and high selectivity. Our work offers a new strategy for rational design of graphene-based materials for detection of OPCs at room temperature.
研究领域:
材料科学
·
化学传感器
·
环境监测
✓ 已验证
产品关联
DOI
高影响因子
Science Bulletin
·
2024
·
IF 18.8
Yida Zhang,Zhentao Ma,Shaokang Yang,Qingyu Wang,Limin Liu,Yu Bai,Dewei Rao,Gongming Wang,Hongliang Li,Xusheng Zheng
Catalytic conversion of nitrate (NO 3 − ) pollutants into ammonia (NH 3 ) offers a sustainable and promising route for both wastewater treatment and NH 3 synthesis. Alkali cations are prevalent in nitrate solutions, but their roles beyond charge balance in catalytic NO 3 − conversion have been generally ignored. Herein, we report the promotion effect of K + cations in KNO 3 solution for NO 3 − reduction over a TiO 2 -supported Ni single-atom catalyst (Ni 1 /TiO 2 ). For photocatalytic NO 3 − reduction reaction, Ni 1 /TiO 2 exhibited a 1.9-fold NH 3 yield rate with nearly 100% selectivity in KNO 3 solution relative to that in NaNO 3 solution. Mechanistic studies reveal that the K + cations from KNO 3 gradually bonded with the surface of Ni 1 /TiO 2 , in situ forming a K-O-Ni moiety during reaction, whereas the Na + ions were unable to interact with the catalyst in NaNO 3 solution. The charge accumulation on the Ni sites induced by the incorporation of K atom promoted the adsorption and activation of NO 3 − . Furthermore, the K-O-Ni moiety facilitated the multiple proton-electron coupling of NO 3 − into NH 3 by stabilizing the intermediates.
研究领域:
环境科学
·
催化化学
·
材料科学
✓ 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）