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
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
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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
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环境科学
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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
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
Journal of Energy Storage
·
2024
·
IF 8.9
Xiling Mao,Hao Liu,Jianhua Xu,Mengwei Li,Wenyao Yang
The rational surface reconstruction of component heterointerfaces is an effective strategy for boosting the electrochemical activity and structural stability of asymmetric supercapacitors. In this study, a Co 3 O 4 /rGO (cobalt oxide/reduced graphene oxide(rGO)) heterostructure was designed using a hydrothermal and annealing strategy. Owing to its abundant electroactive sites, accelerated diffusion reaction kinetics, and strong OH − adsorption capability, the optimized Co 3 O 4 /rGO composite delivered an ultrahigh capacitance of 273.3 F/g at 1 A/g. Additionally, density functional theory (DFT) calculations verified the significant charge transfer from Co 3 O 4 to rGO near the heterointerface, achieving obvious charge redistribution and the formation of a space-charge layer. This optimization enhances significantly optimizes OH − adsorption and diffusion and improves electrical conductivity, leading to the excellent electrochemical performance of the surface-reconstructed Co 3 O 4 /rGO. More importantly, the all-solid-state asymmetric supercapacitor Co 3 O 4 /rGO//AC (activated carbon) demonstrated an exceptional energy density of 16.47 Wh/kg at a power density of 599 W/kg, along with excellent cycling stability, retaining 91.0 % capacitance after 5000 cycles. Overall, this study provides an effective approach for designing surface-reconstructed heterointerfaces to achieve remarkable electrochemical performance and ensure structural integrity, showcasing significant potential for practical applications in the energy storage market.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）