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
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2019
·
IF 14.229
Shujun Qiu,Yongli Shen,Guijuan Wei,Shuang Yao,Wei Xi,Miao Shu,Rui Si,Min Zhang,Junfa Zhu,Changhua An
Maximizing the usage of cocatalyst to provide fruitful proton reduction sites and suppress charge carrier recombination is an effective stratagy to dramatically improve the photocatalytic performance. Herein, anchoring single atoms (SAs) of Pt onto the ultrathin porous CdS@carbon dots (CDs) nanosheets has been achieved through in-situ reduction of Pt precursor. X-ray absorption fine structure spectra identify that the single Pt atoms are bonded as Pt-S with a coordination number 4, due to the scattering between platinum center and the sulfur atoms. The Pt single atoms exhibit strong capacity to trap photo-generated electrons, rendering CdS@CDs/Pt-SAs as a class of efficient solar-driven photocatalyst. It shows an outstanding activity towards H 2 generation at rate of 45.5 mmol h −1 g −1 , which is 133 times of that for bare CdS@CDs. The novel method can be extended to the preparation of various functional nanocatalysts owing to its versatility and facileness.
研究领域:
材料科学
·
纳米技术
·
催化
·
能源材料
✓ 已验证
DOI
高影响因子
Nano Energy
·
2018
·
IF 13.12
Peng Zhou,Fan Lv,Na Li,Yelong Zhang,Zijie Mu,Yonghua Tang,Jianping Lai,Yuguang Chao,Mingchuan Luo,Fei Lin,Jinhui Zhou,Dong Su,Shaojun Guo
Tuning reactive metal-support interaction (RMSI) is a promising approach to optimizing catalytic active sites via the electronic, geometric and compositional effects. In general, the RMSI is conducted on the reducible oxides via a high-temperature reaction (>550 °C). Herein we report a strong RMSI between Pt single atom (PtSA) and non-oxide-based g -C 3 N 4 built by an in-situ photocatalytic reduction method at a sub-zero temperature. The experimental observation confirms that the rich N vacancies in g -C 3 N 4 produce an obvious electron-deficient effect, which greatly enhances the RMSI. This strong RMSI contributes to the highest PtSA coverage density of 0.35 mg m −2 reported to date in carbon-based materials and outstanding H 2 -evolution activity of 174.5 mmol g −1 h −1 per PtSA relative to those on the electron-rich g -C 3 N 4 . The structure simulation reveals that the RMSI can not only stabilize the PtSA on the electron-deficient g -C 3 N 4 via the strong chemical bond between PtSA and the two-coordinated C (C 2C ) sites caused by the N vacancies, but also promises the PtSA with an optimized electronic and geometric structures for capturing photogenerated electrons and producing H 2 . This finding opens a new channel for designing and manipulating single atom-loaded photocatalyst via the RMSI at a sub-zero low temperature.
研究领域:
材料科学
·
催化化学
·
能源科学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Water Process Engineering
·
2024
·
IF 6.3
Nan Zhao,Kangjie Zhang,Yuexiang Lu,Shuang Liu,Zhe Wang,Xiangke Wang
The photocatalytic method has been proven as one of the effective methods for uranium removal from radioactive wastewater. Herein, a photocatalyst UiO-66-NH 2 -Pt was prepared using the adsorption-photoinduction method. Pt was first adsorbed on the substrate and then photo-reduced under light irradiation to be doped into the structure of UiO-66-NH 2 . The characterization results implied the formation and atomic dispersion of Pt with a loading content of 1.90 wt%. The loading of Pt has promoted the effective separation and transfer of photogenerated electron-hole pairs, broadened the visible light adsorption range and narrowed down the bandgap, thus to enhance the photocatalytic activity. Then they were applied for the photo-removal of uranium under air atmosphere. The reaction rate of UiO-66-NH 2 -Pt was about 7 times that of pure UiO-66, confirming the higher photocatalytic activity after the loading of Pt. It showed good reusability and was also universal for different water matrix. The detection of hydroxyl radicals with EPR method indicated the formation of H 2 O 2 , which could react with uranyl ions to form metastudtite under air. This work further verified the feasibility of photoinduced synthesis of Pt single atom and provided a novel material for photocatalytic removal of uranyl ion under air.
研究领域:
环境科学
·
材料科学
·
核工程
✓ 已验证
DOI
高影响因子
ACS Catalysis
·
2021
·
IF 13.084
Yu Gu,Shibin Wang,Huaijie Shi,Jun Yang,Suiqin Li,Haiyang Zheng,Wenbin Jiang,Jia Liu,Xing Zhong,Jianguo Wang
Environment-friendly electrochemical ozone production (EOP) is a promising route for in situ sterilization and discoloration applications. Herein, a Pt-SAs/BNC catalyst with Pt single atoms embedded into B/N codoped nanotubes is rationally designed and prepared. The process provides a local environment rich in oxygen intermediates and hence improves the EOP performance in neutral media by influencing the EOP thermodynamics and kinetics. The Pt-SAs/BNC catalyst exhibits excellent EOP performance with a Faraday efficiency of 21% at the current density of 50 mA cm–2, which is almost twice as much as that of commercial β-PbO2. Density functional theory calculations further reveal the synergistic effect between the B sites and the Pt single atom of the EOP mechanism. In addition, the Pt-SAs/BNC catalyst presented a significant performance in electrodegradation of various pesticides and antibiotics, indicating the potential environmental application capabilities of Pt-SAs/BNC.
研究领域:
材料科学
·
环境科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Hongjie Yu,Wenxin Wang,Qiqi Mao,Kai Deng,Ziqiang Wang,You Xu,Xiaonian Li,Hongjing Wang,Liang Wang
By combining hydrogen evolution reaction (HER) with glycerol oxidation reaction (GOR), high-value chemicals can be obtained at the anode while saving energy to produce hydrogen. Herein, we synthesized Pt SA -NiCo LDHs/NF by anchoring oxygen vacancies in NiCo LDHs with Pt to form Pt-O 5 coordination. Density functional theory (DFT) revealed that Pt SA reduced the d -band center and optimized ΔG H* . During HER, LDHs act as active sites to catalyze H-OH cleavage and promote the dissociation of H 2 O, while Pt single atoms act as the binding sites for H intermediates, and Pt-O bonds accelerate proton-electron coupling and promote the release of H 2 molecules. In HER//GOR, a cell voltage of only 1.37 V is required to provide a current density of 100 mA cm −2 and to produce formate at the anode. This work enables energy-saving hydrogen production and high-value chemicals at the anode, a novel green electrocatalytic synthesis strategy with synergistic coupling and dual promotion.
研究领域:
材料科学
·
能源化学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
Energy & Environmental Science
·
2024
·Vol. 17
·期 14
·5227-5240
·
IF 32.4
Changle Yue,Chao Feng,Guangxun Sun,Na Liu,Haoyuan Hao,Wenjing Bao,Xiaowei Zhang,Fengyue Sun,Cong Zhang,Jiahui Bi,Yan Zhou,Hsiao-Chien Chen,Yuan Pan,Daofeng Sun,Yukun Lu
Tuning and stabilizing the chemical microenvironment of Pt-based single-atom catalysts is a major challenge in promoting an electrocatalytic hydrogen evolution reaction (HER). Herein, we constructed a hierarchical stabilization system of Pt single-atoms via defect substitution using the polyoxometalate (POM) (NH4)4[ZnMo6O24H6] (ZnMo6) as a template. The well-defined structure of ZnMo6 led to precise local Zn sublimation during the formation of Mo2C, which was converted from the Mo6 ring in situ. The localized defect provides a well-defined Mo(C)–Pt–N coordination environment to trap Pt single-atoms. The obtained single-atom catalyst (PtSA@Mo2C@NC) exhibited a superior and stable electrochemical HER performance with an unprecedented mass activity of 75.21 A mgPt−1 in 0.5 M H2SO4. In-depth theoretical calculation analysis revealed that Mo(C)–Pt–N coordination provides a moderated charge state and low d-band center of the Pt site, thus significantly promoting proton adsorption and H2 desorption. This work demonstrates a promising single-atom stabilization strategy for constructing high-performance HER electrocatalysts through the precise modulation of a three-dimensional chemical environment.
研究领域:
材料科学
·
电化学
·
催化
·
能源材料
✓ 已验证
产品关联
DOI
高影响因子
Sustainable Energy & Fuels
·
2020
·Vol. 5
·期 2
·532-539
·
IF 5.503
Zhen Zhang,Cheng Jiang,Ping Li,Qi Feng,Zhi liang Zhao,Keguang Yao,Jiantao Fan,Hui Li,Haijiang Wang
Pt single-atom catalysts (SACs) have shown great potential for electrochemical catalysis. However, no systematic study of their bifunctional catalytic activity for the hydrogen evolution reaction (HER) and the hydrogen oxidation reaction (HOR) has yet been published. More significantly, the reported catalytic capabilities of Pt SACs have almost been exclusively measured using a rotating disk electrode (RDE) with a three-electrode configuration, which does not accurately reflect the catalysts' performance during operation within single-cell devices. Herein, we demonstrate the immobilization of isolated Pt atoms on a carbon nanosheet support doped with ultrahigh N content (12.1 at%; Pt/NCS) to create a bifunctional HER/HOR catalyst. Compared with commercial Pt/C, the developed Pt/NCS catalyst delivered high utilization as well as excellent mass activity enhancement and stability for both reactions. As a final test, a rigorous catalyst evaluation was conducted in both a proton exchange membrane (PEM) electrolyzer and a PEM fuel cell. As expected, with only half the Pt loading of commercial Pt/C, Pt/NCS-based electrodes in the electrolyzer and the fuel cell still exhibited slightly better performance than those based on Pt/C. This work constitutes a huge step from the academic study of Pt-based SCAs to their industrial application, and it focuses more attention on the harsh evaluation and optimization of SACs within commercial-scale devices.
研究领域:
电化学
·
材料科学
·
催化
·
能源存储与转换
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Nano Materials
·
2024
·
IF 5.3
Yong Zhang,Xin Zeng,YiYi Liu,Cuncun Wang,Changpeng Jin,Jingzhou Hou,Mei Yang,Danqun Huo
Developing an accurate, reliable, and stable glucose detection sensor poses a formidable challenge for the food industry. In this study, hydrothermal and wet chemical methods were employed to fabricate a Pt single-atom catalyst on Co3O4 (Co3O4/Pt SAs), where dispersed Pt atoms collaboratively catalyze the electrochemical reaction on the electrode surface. Subsequently, the integration of the microelectrode with polyethylene glycol diacrylate (PEG-DA) hydrogel and a dual-channel microfluidic chip facilitated continuous and rapid glucose detection. The addition of 5% PEG-DA hydrogel served to eliminate interference and expedite glucose detection, while the design of the dual-channel microfluidic chip generated microscale vortices, providing ample reaction opportunities for the target glucose while preventing interference from the mixing of previous and current reaction solutions. The research exhibited a favorable linear detection range from 1 to 800 μM, with a detection limit of 0.84 μM. Furthermore, validation of the device’s feasibility in real samples demonstrated a glucose recovery rate ranging from 94.9 to 104.4% in beverages.
研究领域:
电化学
·
材料科学
·
分析化学
·
生物技术
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）