ACS Catalysis
·
2021
·
IF 13.084
Kaili Wang,Danyang Huang,Yichi Guan,Feng Liu,Jia He,Yi Ding
Designing highly efficient and durable electrocatalysts for methanol oxidation reaction (MOR) plays a decisive role in the commercialization of direct methanol fuel cells (DMFCs). Compared with commercial Pt/C catalysts, fine-tuning the electronic structure of electrocatalysts to reduce the adsorption energy of CO while at the same time increasing the adsorption energy of OH is beneficial to improving the activity of MOR. Herein, ultrastable self-supported PtCu nanowires (NWs) with abundant Cu-vacancies have been developed, wherein the CO adsorption energy is weakened by doping of Cu elements and the OH adsorption energy is strengthened by the vacancy defect through dealloying. The well-designed PtCu NWs exhibit an outstanding performance for the MOR, with a specific activity 7.5 times higher than that for the commercial Pt/C catalyst, which transcends most electrocatalysts’ performance currently. Moreover, the stability of PtCu electrocatalysts is greatly improved over 1 h owing to a “non-CO” pathway for MOR. Further DMFC tests present a 2 times higher power density than that of commercial Pt/C, and the PtCu integrated DMFC also presents a higher stability for 24 h, transcending most Pt-based anode catalysts of DMFCs.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Nano Materials
·
2022
·
IF 6.14
Zi-Yao Chen,Wen-Zhu Shao,Wei-Jian Li,Xue-Yin Sun,Liang Zhen,Yang Li
Due to the strong surface energy and polarity, ZnO nanoparticles are prone to adsorbing the OH groups dissociated from water in the air, leading to easy agglomeration and hence deteriorating the dispersion of ZnO in composites. In this work, it has been theoretically and experimentally demonstrated that doping with lower electronegativity metallic ions is an effective strategy to suppress the agglomeration of ZnO nanoparticles. By calculating the adsorption energies and electronic structures of OH/M-doped ZnO configurations (M = Li+, Cu2+, Al3+), it was found that metallic ion doping with a lower electronegativity (in comparison to that of the host Zn2+) can efficiently reduce the adsorption of OH groups on the ZnO surface due to the lower effective bond order of M–O bonds. Guided by the theoretical results, various M-doped ZnO nanoparticles (M = Li+, Cu2+, Al3+) were prepared and characterized by X-ray photoelectron spectroscopy and a laser particle sizer, which confirmed that the lower the electronegativity of dopants, the lower the OH groups’ adsorbed amounts and aggregate sizes of M-doped ZnO nanoparticles. This work provides a general avenue to design the composition of M-doped ZnO nanoparticles for suppressing agglomeration and enhance the dispersion of ZnO in composites.
研究领域:
材料科学
·
表面化学
✓ 已验证
DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2022
·
IF 10.319
Xiumei Chen,Na Xin,Yuxin Li,Cong Sun,Longhua Li,Yulong Ying,Weidong Shi,Yu Liu
The energy storage device has been urgently studied and developed to meet the increasing demand for energy and sustainable development. Due to the excellent conductivity of graphene and high performance of ZnCo 2 O 4 and NiCo 2 O 4 , we design a self-supporting electrode based on vertically grown two-dimensional/two-dimensional (2D/2D) NiCo 2 O 4 /ZnCo 2 O 4 hierarchical flakes on the carbon-based conductive substrate (NiCo 2 O 4 /ZnCo 2 O 4 @graphene/carbon nanotubes, NZ@GC). The density functional theory calculations indicate that the high OH − adsorption capacity of the NiCo 2 O 4 /ZnCo 2 O 4 nanosheets can significantly enhance the electrochemical reaction activity. NZ@GC shows a high capacitance of 1128.6 F g −1 at 1 A g −1 . The capacitance retains 84.0% after 6000 cycles even at 10 A g −1 . A hybrid supercapacitor is fabricated using NZ@GC and activated carbon, exhibiting a large energy density of 50.8 W h kg −1 at the power density of 800 W kg −1 . After 9000 charge/discharge cycles, the supercapacitor still has 86.1% capacitance retention. The NZ@GC film has showed the potential as promising electrodes in high efficiency electrochemical energy storage devices.
研究领域:
材料科学
·
能源存储
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Yuechao Yang,Danxia Xu,Baolong Zhang,Zhimin Xue,Tiancheng Mu
Electrochemical oxidation of alcohol and aldehyde to carboxylic acids is one of the most important classes of catalytic reaction. The key point for such reactions lies in the fine tailoring the catalysts to improve the reaction and energy efficiency. For such a destination, identifying descriptors which are highly related to the catalytic efficiency is a prerequisite for designing electrocatalysts. In this work, taking 5-hydroxymethylfurfural (HMF), a biomass derived platform molecule containing alcohol and aldehyde, as the main research object, we revealed for the first time that the adsorption energy of substrate molecule is an activity descriptor for electrochemical alcohol and aldehyde oxidation. Too weak substrate adsorption is not favorable to C–H/O–H bond activation and dissociation, while too strong substrate adsorption hinders the formation of enough OH ads (an important intermediate) due to the competitive adsorption of substrate molecules and OH – at limited reaction sites. The optimal catalytic activity can be achieved by adjusting the adsorption energy of substrate molecules to make them properly adsorbed on the catalyst surface. This work not only offers a guideline for the design of advanced catalysts towards the electrochemical alcohol and aldehyde oxidation (e.g., methanol, ethanol, benzyl alcohol, glycerol, glucose, furfural and HMF) for the utilization and production of renewable resources, but also benefits the design of other electrochemical catalysts.
研究领域:
电化学
·
催化
·
可再生能源
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2025
·
IF 17.7
Zhouzhou Wang,Qiancheng Zhou,Li Luo,Yaran Shi,Haoran Li,Chunchun Wang,Kesheng Lin,Chengsi Wang,Libing Zhu,Linyun Han,Zhuo Xing,Ying Yu
Neutral oxygen evolution reaction (OER) is a crucial half-reaction for electrocatalytic chemical production under mild condition, but with limited development due to low activity and poor stability. Herein, a tungsten-doped cobalt molybdate (WDCMO) catalyst was synthesized for efficient and durable OER under neutral electrolyte. It is demonstrated that catalyst reconstruction is suppressed by W doping, which stabilizes the Co-O-Mo point-to-point connection in CoMoO 4 architecture and stimulates to a lower valence state of active sites over the surface phase. Thereby, the surface structure maintains to avoid compound dissolution caused by over-oxidation during OER. Meanwhile, the WDCMO catalyst promotes charge transfer and optimizes *OH intermediate adsorption, which improves reaction kinetics and intrinsic activity. Consequently, the WDCMO electrode exhibits an overpotential of 302 mV at 10 mA cm –2 in neutral electrolyte with an improvement of 182 mV compared with CoMoO 4 electrode. Furthermore, W doping significantly improves the electrode stability from 50 h to more than 320 h, with a suppressive potential attenuation from 2.82 to 0.29 mV h –1 . This work will shed new light on designing rational electrocatalysts for neutral OER.
研究领域:
电化学
·
催化
·
材料科学
·
能量转换
·
纳米技术
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Dan Li,Zuquan Gan,Cailin Zhang,Xiuqiu Wang,Mingzhen Zheng,Xiaoyun Gao,Yue Huang,Youjun Fan,Shuifeng Zhang,Fuqin Zheng,Wei Chen
The exploration of sustainable approaches for plastic waste disposal has emerged as an urgent imperative task. This research presents an innovative and eco-friendly electrochemical route to degrade plastic waste, ethylene glycol (EG), into value-added formate. To this end, an interesting hollow FeOOH/CoOOH heterostructure is successfully fabricated for EG oxidation. The difference in work functions between FeOOH and CoOOH results in the establishment of a built-in electric field (BEF), which is beneficial for the adsorption of EG and *OH. As a result, the FeOOH/CoOOH demonstrates outstanding catalytic performance in the EG oxidation reaction (EGOR) with an exceptionally low potential of only 1.32 V at 10 mA cm -2 and a high Faraday efficiency of 92.19% for formate generation. Glycollic acid is identified as a pivotal intermediate in the EGOR by in-situ infrared spectroscopy. Theoretical computations disclose that the FeOOH/CoOOH heterostructure not only causes an upward shift of the d-band center but also largely enhances the *OH adsorption, thus speeding up the cleavage of the inert C-C bond and markedly facilitating the conversion of EG to formate. This research not only enriches the fundamental comprehension of the EGOR but also provides deep insights for the rational design of highly selective and active EGOR catalysts.
研究领域:
电化学
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催化
·
材料科学
·
环境科学
·
纳米技术
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
INORGANIC CHEMISTRY
·
2022
·
IF 5.436
Qianqian Wu,Xin Huang,Tingting Wan,Dong Xiang,Xiaowu Li,Kun Wang,Xiaoyou Yuan,Peng Li,Manzhou Zhu
A key challenge for direct methanol fuel cells is the sluggish reaction kinetics, poor anti-CO poisoning ability, and insufficient Pt utilization of platinum-based catalysts during methanol oxidation reaction (MOR). Herein, we report a facile approach for PtCuNi electrocatalysts with adjustable inner and surface configurations. By judiciously controlling the nucleation/growth kinetics, PtCuNi core–shell alloy nanoparticles (PtCuNi-CS NPs) fortified with a Cu-rich core and a Pt-rich shell are obtained. Especially, PtCuNi-CS NPs show the highest mass activity and specific activity toward MOR, 5.7 and 5.1 times higher than those of commercial Pt/C. Density functional theory calculations reveal that the PtCuNi-CS NPs with a suitable d-band center possess excellent electro-oxidation activity. Additionally, the doping of Cu and Ni atoms endows the PtCuNi-CS NPs with enhanced OH* adsorption. This work provides an effective design strategy to develop Pt-based trimetallic electrocatalysts as efficient anode materials for fuel cell applications.
研究领域:
电化学
·
材料科学
·
催化
·
能源材料
✓ 已验证
DOI
高影响因子
Nature Communications
·
2025
·Vol. 16
·期 1
·1-11
·
IF 15.7
He Xun,Yao Yongchao,Zhang Min,Zhou Yilei,Zhang Limei,Ren Yuchun,Dong Kai,Tang Hong,Nan Jue,Zhou Xingli,Luo Han,Ying Binwu,Yu Qi,Luo Fengming,Tang Bo,Sun Xuping
Seawater electrolysis driven by offshore renewable energy is a promising avenue for large-scale hydrogen production but faces challenges in designing robust anodes that suppress surface chlorine reactions and corrosion at high current densities. Here we report a strategy by selectively docking PW 12 -polyoxometalate (PW 12 -POM) onto Fe sites of CoFe hydroxide anode to modulate the electronic structure of adjacent Co active centers and regulate Cl⁻/OH⁻ adsorption for efficient alkaline seawater oxidation. Our CoFe-based anode achieves low overpotentials, high catalytic selectivity, and notable durability, with continuous operation at 1 A cm⁻² for over 1300 hours and at 2 A cm⁻² more than 600 hours. Theoretical calculations and ex situ/in situ analyses reveal that PW 12 -POM coordination at Fe sites stabilizes Fe, suppresses its leaching, modulates Co acidity, promotes OH⁻ adsorption, and protects metal sites from Cl⁻ corrosion.
研究领域:
电化学
·
材料科学
·
能量转换
·
催化
·
可再生能源
·
表面化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
DALTON TRANSACTIONS
·
2021
·Vol. 50
·期 28
·9746-9753
·
IF 4.39
Yan He,Tao Yu,Hui Wen,Rui Guo
For the electrocatalytic oxygen evolution reaction (OER) in alkaline media, there is an urgent need to optimize the adsorption strength of OH*. Here, a flower-like hybrid of Cr-doped FeOOH/Ni(OH)2 was used as an OER catalyst with a low overpotential of 291 mV at 50 mA cm−2. The results showed that faster charge transfer was achieved at the electrode/solution interface during the OER process after the FeOOH/Ni(OH)2 was modified by Cr, which facilitates the rate-determining step of the Volmer reaction. Furthermore, the results of faradaic efficiency and X-ray photoelectron spectroscopy (XPS) measurements confirmed that the synergistic effect between the ternary metal and oxygen vacancies led to excellent OER performance. This work provides a new strategy for the preparation of high-efficiency and low-cost oxygen evolution electrocatalysts.
研究领域:
电化学
·
材料科学
·
催化
·
能源材料
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-10
·
IF 14.7
Lv Jiabao,Cao Ang,Zhong Yunhao,Lin Qingyang,Li Xiaodong,Wu Hao Bin,Yan Jianhua,Wu Angjian
Renewable-driven electrocatalytic nitrate conversion offers a promising alternative to alleviate nitrate pollution and simultaneously harvest green ammonia. However, due to the complex proton-electron transfer processes, the reaction mechanism remains elusive, thereby limiting energy efficiency. Here, we adopt Ni(OH)₂ as a model catalyst to investigate the dynamic evolution of the reaction interface. A proposed OH cycle mechanism involves the formation of a locally OH-enriched microenvironment to promote the hydrogenation process, which is identified through in-situ spectroscopy and isotopic labelling. By further activating the dynamic state through the implementation of surface vacancies via plasma, we achieve a high Faradaic efficiency of almost 100%. The activated interface accelerates the OH cycle by enhancing dehydroxylation, water dissociation, and OH adsorption, thereby promoting nitrate electroreduction and inhibiting hydrogen evolution. We anticipate that rational activation of the dynamic interfacial state can facilitate electrocatalytic interface activity and improve reaction efficiency.
研究领域:
电化学
·
催化
·
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
Nature Catalysis
·
2022
·Vol. 5
·期 10
·900-911
·
IF 40.706
Li Peng,Jiang Yaling,Hu Youcheng,Men Yana,Liu Yuwen,Cai Wenbin,Chen Shengli
The origin of the large kinetic pH effect in hydrogen electrocatalysis, that is, the approximately two orders of magnitude decrease in reaction kinetics when moving from acid to alkaline, remains far from having a consensus. Here we show that it is the significantly different connectivity of hydrogen-bond networks in electric double layers that causes the large kinetic pH effect. This result has been obtained by meticulously comparing the electric double layers of acid and alkaline interfaces from ab initio molecular dynamics simulations, and the computed vibrational density of states of water molecules in the interfaces simulated with ab initio molecular dynamics, with the results of in situ surface-enhanced infrared absorption spectroscopy. Using a Pt–Ru alloy as a model catalyst, we further reveal an unanticipated role of OH adsorption in improving the kinetics of alkaline hydrogen electrocatalysis, namely, by increasing the connectivity of hydrogen-bond networks in electric double layers rather than by merely affecting the energetics of surface reaction steps. These findings highlight the key roles of electric double layer structures in electrocatalysis.
研究领域:
电化学
·
催化
·
材料科学
·
表面科学
✓ 已验证
DOI
高影响因子
Nano Research
·
2020
·Vol. 13
·期 12
·3292-3298
·
IF 8.183
Wei Pengkun,Hao Zewei,Yang Yang,Liu Mingyang,Zhang Haijun,Gao Min-Rui,Yu Shu-Hong
Although nickel-based catalysts display good catalytic capability and excellent corrosion resistance under alkaline electrolytes for water splitting, it is still imperative to enhance their activity for real device applications. Herein, we decorated Ni 0.85 Se hollow nanospheres onto reduced graphene oxide (RGO) through a hydrothermal route, then annealed this composite at different temperatures (400 °C, NiSe 2 -400 and 450 °C, NiSe 2 -450) under argon atmosphere, yielding a kind of NiSe 2 /RGO composite catalysts. Positron annihilation spectra revealed two types of vacancies formed in this composite catalyst. We found that the NiSe 2 -400 catalyst with dual Ni-Se vacancies is able to catalyze the oxygen evolution reaction (OER) efficiently, needing a mere 241 mV overpotential at 10 mA·cm −2 . In addition, this catalyst exhibits outstanding stability. Computational studies show favorable energy barrier on NiSe 2 -400, enabling moderate OH − adsorption and O 2 desorption, which leads to the enhanced energetics for OER.
研究领域:
材料科学
·
电化学
·
催化
·
纳米技术
✓ 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）