Communications Chemistry
·
2019
·Vol. 2
·期 1
·1-11
·
IF 0
Sun Xiucheng,Lin Jian,Chen Yang,Wang Yuehan,Li Lin,Miao Shu,Pan Xiaoli,Wang Xiaodong
Minimizing the use of precious metal remains a challenge in heterogeneous catalysis, such as platinum-based catalysts for formaldehyde oxidation. Here we report the catalyst system Pt/TiO 2 with low platinum loading of 0.08 wt%, orders of magnitude lower than conventional catalysts. A volcano-like relationship is identified between reaction rates of formaldehyde and platinum sizes in a scale of single-atoms, nanoclusters and nanoparticles, respectively. Various characterization techniques demonstrate that platinum nanoclusters facilitate more activation of O 2 and easier adsorption of HCHO as formates. The activated O facilitates the decomposition of formates to CO 2 via a lower reaction barrier. Consequently, this size platinum with such low loading realizes complete elimination of formaldehyde at ambient conditions, outperforming single-atoms and nanoparticles. Moreover, the platinum nanoclusters exhibit a good versatility regardless of supporting on “active” FeO x or “inert” Al 2 O 3 for formaldehyde removal. The identification of the most active species has broad implications to design cost-effective metal catalysts with relatively lower loadings.
研究领域:
催化化学
·
环境科学
✓ 已验证
产品关联
DOI
CHINESE JOURNAL OF CATALYSIS
·
2025
·
IF 17.7
Jiaxin Li,Yan Lv,Xueyan Wu,Xinyu Guo,Zhuojun Yang,Jixi Guo,Tianhua Zhou,Dianzeng Jia
To address the high cost and limited electrochemical endurance of Pt-based electrocatalysts, the appropriate introduction of transition metal-based compounds as supports to disperse and anchor Pt species offers a promising approach for improving catalytic efficiency. In this study, sub-1 nm Pt nanoclusters were uniformly confined on NiO supports with a hierarchical nanotube/nanosheet structure (Pt/NiO/NF) through a combination of spatial domain confinement and annealing. The resulting catalyst exhibited excellent electrocatalytic activity and stability for hydrogen evolution (HER) and urea oxidation reactions (UOR) under alkaline conditions. Structural characterization and density functional theory calculations demonstrated that sub-1 nm Pt nanoclusters were immobilized on the NiO supports by Pt–O–Ni bonds at the interface. The strong metal-support interaction induced massive charge redistribution around the heterointerface, leading to the formation of multiple active sites. The Pt/NiO/NF catalyst only required an overpotential of 12 and 136 mV to actuate current densities of 10 and 100 mA cm −2 for the HER, respectively, and maintained a voltage retention of 96% for 260 h of continuous operation at a current density of 500 mA cm −2 . Notably, in energy-efficient hydrogen production systems coupled with the HER and UOR, the catalyst required cell voltages of 1.37 and 1.53 V to drive current densities of 10 and 50 mA cm −2 , respectively—approximately 300 mV lower than conventional water electrolysis systems. This study presents a novel pathway for designing highly efficient and robust sub-nanometer metal cluster catalysts.
研究领域:
材料科学
·
能源化学
✓ 已验证
产品关联
DOI
高影响因子
ANALYST
·
2019
·Vol. 144
·期 17
·5179-5185
·
IF 4.019
Xiaolei Guo,Yixing Suo,Xuan Zhang,Yanshuai Cui,Shengfu Chen,Haotian Sun,Dawei Gao,Zhiwei Liu,Longgang Wang
The development of noble ultra-small biocompatible Pt nanoclusters (Pt NCs) for glucose detection has been drawing great attention. Herein, ultra-small biocompatible jujube polysaccharide (JP) stabilized platinum nanoclusters (Ptn-JP NCs) are prepared using natural JP as a reducing and solubilizing agent. Ptn-JP NCs were studied for the colorimetric detection of glucose. Ptn-JP NCs (n = 50, 200 and 400) had an average particle diameter of 1–2 nm. Particularly, the measurements of hydrodynamic sizes of Ptn-JP NCs indicated that they maintained good stability in solution for one week. Pt200-JP NCs showed good biocompatibility, and were not toxic against HeLa cells at a high concentration of 400 μg mL−1. Furthermore, Pt200-JP NCs catalyzed the oxidation of 3,3′,5,5′-tetramethylbenzidine (TMB) with H2O2 to produce blue oxidized TMB (oxTMB). This reaction followed typical Michaelis–Menten kinetics. More importantly, the glucose concentration could be sensitively detected by the color change, and this process was not interfered by other sugars. The linear range for glucose concentration was from 0.01 to 1 mM with a detection limit of 5.47 μM. The glucose concentrations of real samples of serum using Pt200-JP NCs were 9.2, 4.9 and 6.5 mM, respectively. The prepared Ptn-JP NCs have great potential in various biomedical detection methods.
研究领域:
生物医学
·
材料科学
·
分析化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
INORGANIC CHEMISTRY
·
2021
·
IF 5.165
Zhiyang Zhang,Gui Liu,Liping Ding,Mi Hu,Jing Gu,Wenlong Xu,Qingbo Xiao
The microenvironment surrounding the metal clusters on a carrier produces a tremendous influence on its catalytic performance. In this work, the promotion effect of the zeolitic inner host on catalytic performance of encapsulated platinum nanoclusters is reported. In the reaction of phenylacetylene semihydrogenation to styrene, Pt@X-zeolite, where platinum nanoclusters are encapsulated into the inner microporosity of the X-zeolite, exhibits an ∼3.37 times increased turnover frequency and a much better selectivity of 87.6% in comparison to the referenced Pt/X-zeolite of 79.3% selectivity to styrene at the same reaction conditions, in which the platinum nanoclusters are located at the exterior of the zeolite. Meanwhile, the Pt@X-zeolite displays a higher stability after 10 cycles of the reaction. Through the detailed characteristics, the excellent performance of Pt@X-zeolite is mainly due to the promotion of the zeolitic framework on the encapsulated Pt clusters, resulting in “electron-deficient” Pt clusters, leading to a stronger interaction with the π* molecular orbitals of phenylacetylene and thus enhancing the activation and conversion of phenylacetylene. The zeolite cavity wrapped with encapsulated Pt clusters regulates the adsorption trend of phenylacetylene through the acetylene group on it, promotes the desorption of styrene, and strengthens its selectivity. Meanwhile, Pt@X-zeolite has an excellent stability through the zeolite framework, which protects the Pt species from being lost. This investigation reveals the importance of the zeolitic microenvironment on the catalytic performance of encapsulated metal species and deepens the cognition for this type of catalyst.
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
ELECTROCHIMICA ACTA
·
2018
·
IF 5.116
Cheng Du,Xiaohui Gao,Chunfeng Cheng,Zhihua Zhuang,Xiaokun Li,Wei Chen
Metal nanoclusters have attracted increasing attentions due to their extremely high catalytic activities. However, how to keep their structural and catalytic stabilities is still a challenge, especially in electrocatalysis . Herein, a novel mutual-interacted Pt CeO 2 C ternary nanostructure was designed and fabricated from Ce-based metal organic framework (Ce-MOF). In this unique nanostructure, through a calcination process, abundant tiny CeO 2 nanoclusters (∼2 nm) can be produced from the Ce-MOF itself and they are uniformly inserted in the MOF-derived porous carbon matrix. Meanwhile, the following deposited surfactant-free Pt nanoclusters (∼2 nm) contact well with both carbon and CeO 2 nanoclusters. The electrocatalytic activity of the Pt CeO 2 C ternary nanostructure for the oxygen reduction reaction (ORR) was investigated. With such ternary structure, the interacted CeO 2 and Pt nanoclusters showed high stability. Moreover, the CeO 2 can modify the electronic density of Pt and enhance the interaction between Pt and carbon at the Pt CeO 2 interface. Meanwhile, with the mutual interaction, the corrosion resistance of carbon can be improved at the CeO 2 C interface, and the conductivity of the catalyst can be improved with the carbon framework. With these structure advantages, the Ce-MOF-derived catalyst exhibited higher electrocatalytic performance than commercial Pt C for ORR with more positive half-wave potential and higher limiting diffusion current density. The origin of the enhanced ORR performance was further disclosed by X-ray absorption fine spectroscopy (XAFS) characterization.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
Small
·
2024
·
IF 13
Guilin Wei,Linsen Zhou,Xianglin Wang,Ru Tang,Kelin Chen,Junhong Luo,Jiangfeng Song,Yan Shi,Ning Liu,Xingwen Feng
The construction, use, and maintenance of tritium-related equipment will inevitably produce tritium-containing radioactive waste gas, and the production of efficient catalysts for tritium removal remains a difficult problem. Herein, silicalite-1 zeolite with entrapped Pt nanoclusters is skillfully post-oxidized at an appropriate temperature, building highly active Pt─O sites on the nanoclusters to achieve efficient oxidation of hydrogen isotopes at low temperatures. The designed Pt─O sites can directly participate in the oxidation reaction of hydrogen isotopes. Compared to the case without Pt─O sites, the presence of these sites significantly reduces the reaction energy barrier to 0.55 eV, enabling the catalyst to achieve a hydrogen conversion rate of 99% at a low temperature of 40 °C. Specifically, the O atoms consumed by the Pt─O sites in the reaction are replaced by O 2 gas and this cycle repeats, which is consistent with the Mars-van Krevelen (M–K) theory. This ensures efficient catalytic oxidation of hydrogen isotopes, and provides an astonishingly high conversion rate of 99% in the nearly 34 days restart performance test. The results of this study provide insights into the strategic design of efficient catalysts for hydrogen isotope oxidation.
研究领域:
催化化学
·
核能科学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2015
·
IF 6.723
Tao Yang,Guojian Cao,Qingli Huang,Yanxia Ma,Sheng Wan,Hong Zhao,Na Li,Xia Sun,Fujun Yin
Exploring superior catalysts with high catalytic activity and durability is of significant for the development of an electrochemical device involving the oxygen reduction reaction. This work describes the synthesis of Pt-on-Pd bimetallic heterogeneous nanostructures, and their high electrocatalytic activity toward the oxygen reduction reaction (ORR). Pt nanoclusters with a size of 1–2 nm were generated on Pd nanorods (NRs) through a modified Cu underpotential deposition (UPD) process free of potential control and a subsequent surface-limited redox reaction. The Pt nanocluster decorated Pd nanostructure with a ultralow Pt content of 1.5 wt % exhibited a mass activity of 105.3 mA mg–1 (Pt–Pd) toward ORR, comparable to that of the commercial Pt/C catalyst but 4 times higher than that of carbon supported Pd NRs. More importantly, the carbon supported Pt-on-Pd catalyst displays relatively small losses of 16% in electrochemical surface area (ECSA) and 32% in mass activity after 10 000 potential sweeps, in contrast to respective losses of 46 and 64% for the commercial Pt/C catalyst counterpart. The results demonstrated that Pt decoration might be an efficient way to improve the electrocatalytic activity of Pd and in turn allow Pd to be a promising substitution for commercial Pt catalyst.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Advanced Science
·
2025
·
IF 14.1
Guilin Wei,Jiangfeng Song,Yan Shi,Linsen Zhou,Xianglin Wang,Junhong Luo,Ning Liu,Feize Li,Xingwen Feng
Catalytic oxidation plays a crucial role in the efficient treatment of hydrogen isotopes, with the key technical challenge being the development of high-performance catalysts to enhance isotope removal efficiency, thereby reducing environmental pollution and ensuring public radiation safety. Herein, the strategic control of platinum nanoclusters confined within silicalite-1 zeolites is reported to enhance the high removal efficiency for hydrogen isotopes under low-temperature conditions for the first time. Incorporating a single lanthanum oxide (LaO x ) into Pt nanoclusters adapts the local charge of adjacent Pt atoms, significantly altering their electronic structure. The existence of individual LaO x species is confirmed by X-ray absorption spectroscopy and aberration-corrected electron microscopy, and the performance enhancement mechanism is further probed by theoretical calculations. This embedded single LaO x both facilitates local charge adjustment and supplies abundant active oxygen species, leading to performance enhancement by reducing the energy barrier of rate-determining step (O * + H → OH * ), in accordance with the Mars-van Krevelen mechanism. Consequently, during a surprisingly long-term restart performance test (≈267 d), the PtLaOx@S-1 maintained a high conversion rate over 99% at 50 °C and a space velocity of 48,000 mL·g −1 ·h −1 . This study highlights the potential of individual LaO x sites for enhancing hydrogen isotope oxidation.
研究领域:
催化化学
·
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Nano Research
·
2021
·Vol. 15
·期 4
·3065-3072
·
IF 8.897
Du Peng,Huang Kai,Fan Xiaoyuan,Ma Jingteng,Hussain Naveed,Wang Ruyue,Deng Bohan,Ge Binghui,Tang Haolin,Zhang Ru,Lei Ming,Wu Hui
Being a typical state of the art heterogeneous catalyst, supported noble metal catalyst often demonstrates enhanced catalytic properties. However, a facile synthetic method for realizing large-scale and low-cost supported noble metal catalyst is strictly indispensable. To this end, by making use of the strong metal-support interaction (SMSI) and mechanochemical reaction, we introduce an efficient synthetic route to obtain ultrafine Pt and Ir nanoclusters immobilized on diverse substrates by wet chemical milling. We further demonstrate the scaling-up effect of our approach by large-scale ball-milling production of Pt nanoclusters immobilized on TiO 2 substrate. The synthesized Pt/Ir@Co 3 O 4 catalysts exhibit superior oxygen evolution reaction (OER) performance with only 230 and 290 mV overpotential to achieve current density of 10 and 100 mA·cm −2 , beating the catalytic performance of Co 3 O 4 supported Pt or Ir clusters and commercial Ir/C. It is envisioned that the present work strategically directs facile ways for fabricating supported noble metal heterogeneous catalysts.
研究领域:
材料科学
·
催化化学
✓ 已验证
DOI
高影响因子
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2021
·
IF 6.953
Le Dong,Ruyu Li,Liqiu Wang,Xifa Lan,Haotian Sun,Yu Zhao,Longgang Wang
The sensitive colorimetric detection of glucose using nanomaterials has been attracting considerable attention. To improve the detection sensitivity, highly stable lentinan stabilized platinum nanoclusters (Pt-LNT NCs) were prepared, in which lentinan was employed as a mild reductant and stabilizer. The size of platinum nanoclusters (Pt NCs) was only 1.20 ± 0.29 nm. Pt-LNT NCs catalyzed the oxidation of substrate 3,3′,5,5′-tetramethylbenzidine (TMB) in the presence of hydrogen peroxide (H 2 O 2 ) to produce a blue oxidation product with absorption peak at 652 nm, indicating their peroxidase-like properties. Their enzymatic kinetics followed typical Michaelis-Menten theory. In addition, fluorescence experiments confirmed their ability to efficiently catalyze the decomposition of H 2 O 2 to generate •OH, which resulted in the peroxidase-like mechanism of Pt-LNT NCs. Moreover, a colorimetric method for highly selective and sensitive detection of glucose was established by using Pt-LNT NCs and glucose oxidase. The linear range of glucose detection was 5–1000 μM and the detection limit was 1.79 μM. Finally, this method was further used for detection of glucose in human serum and human urine. The established colorimetric method may promote the development of biological detection and environmental chemistry in the future.
研究领域:
生物化学
·
纳米医学
·
分析化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Materials Research and Technology-JMR&T
·
2020
·
IF 5.289
Liang Li,Ya Yang,Yaowei Wang,Manli Liang,Yuanxing Huang
Suitable electrode catalyst is a critical factor for the application of direct methanol fuel cell. In this research, layered double hydroxides (LDH) are chosen as the supporting material for platinum to improve its electrochemical activity, tolerance to carbonaceous intermediates as well as reduce the cost of electrode. Experimental results show that low amount of platinum (42 and 29 mg/g) can be intercalated into the interlayer of LDH with a thickness less than 1 nm, which can effectively enhance the electrochemical activity as well as reduced the cost. Both MgAl-LDH/Pt and NiFe-LDH/Pt have a lower onset potential toward methanol oxidation than commercial 20% Pt/C. In addition, the peak current of NiFe-LDH/Pt is 18.0 mA/cm 2 , which is 1.5- and 4.7-fold higher than that of MgAl-LDH/Pt and commercial 20% Pt/C, respectively. MgAl-LDH/Pt has a higher tolerance to CO poisoning due to its preference to the generation of hydroxyl radical rather than oxygen evolution reaction, which is commonly observed on the surface of NiFe-LDH. By using electrochemical impedance spectroscopy technique, it can be observed that the intercalation of Pt could effectively reduce the electron transfer resistance of LDH.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
ANALYTICA CHIMICA ACTA
·
2016
·
IF 4.712
Na Xu,Hong-Wei Li,Yuqing Wu
A novel one-step hydrothermal synthesis of highly fluorescent platinum nanoclusters protected by polyethylenimine (Pt-NCs@PEI) is described. The products are characterized well by UV–vis absorption, fluorescence spectra , X-ray photoelectron spectroscopy (XPS) and transmission electron microscopy (TEM) imaging. The Pt-NCs@PEI possess high quantum yield at 28%, which is the relatively high one among the reported Pt-NCs; especially, the synthesis is in one-step and the reaction time is much shorter (<1 h) than the related methods. In addition, the Pt-NCs@PEI have large Stocks-shift (∼150 nm), high tolerability to the extreme pH and high ionic strengths , and excellent photo-stability under UV–vis irradiation, lay the foundation for the practical bio-applications. Finally, the obtained Pt-NCs@PEI are used to determine trace amount of metronidazole (MTZ) in buffer solution in showing a linear response over a concentration range of 0.25–300 μM and a low detection limit of 0.1 μM. Furthermore, the related investigation on response mechanism will be helpful to design and synthesize new metal nanoclusters as fluorescent probe to detect the trace amount of harmful medicine residuum as nitroimidazoles in human body.
研究领域:
分析化学
·
纳米材料科学
·
生物医学工程
✓ 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）