Molybdenum carbide(Mo_(2)C)is a promising non-noble metal electrocatalyst with electronic structures similar to Pt for hydrogen evolution reaction(HER).However,strong H^(*)adsorption at the Mo sites hinders the improv...Molybdenum carbide(Mo_(2)C)is a promising non-noble metal electrocatalyst with electronic structures similar to Pt for hydrogen evolution reaction(HER).However,strong H^(*)adsorption at the Mo sites hinders the improvement of HER performance.Here,we synthesized monodisperse hollow Mo_(2)C nanoreactors,in which the carbon dots(CD)were in situ formed onto the surface of Mo_(2)C through carburization reactions.According to finite element simulation and analysis,the CD@Mo_(2)C possesses better mesoscale diffusion properties than Mo_(2)C alone.The optimized CD@Mo_(2)C nanoreactor demonstrates superior HER performance in alkaline electrolyte with a low overpotential of 57 mV at 10 mA cm^(−2),which is better than most Mo_(2)C-based electrocatalysts.Moreover,CD@Mo_(2)C exhibits excellent electrochemical stability during 240 h,confirmed by operando Raman and X-ray diffraction(XRD).Density functional theory(DFT)calculations show that carbon dots cause the d-band center of CD@Mo_(2)C to shift away from Fermi level,promoting water dissociation and the desorption of H^(*).This study provides a reasonable strategy towards high-activity Mo-based HER eletrocatalysts by modulating the strength of Mo–H bonds.展开更多
针对多重同步挤压变换及其改进算法存在的未重排点问题,提出了一种基于最大系数的多重同步挤压变换(maximum coefficient based multi-synchrosqueezing transform,简称MCMSST)方法来识别时变结构非平稳响应信号的瞬时频率(instantaneou...针对多重同步挤压变换及其改进算法存在的未重排点问题,提出了一种基于最大系数的多重同步挤压变换(maximum coefficient based multi-synchrosqueezing transform,简称MCMSST)方法来识别时变结构非平稳响应信号的瞬时频率(instantaneous frequency,简称IF)。首先,引入傅里叶频谱来辅助多分量响应信号选取截止频率;其次,对响应信号进行短时傅里叶变换(short time fourier transform,简称STFT),针对短时傅里叶变换系数求取针对时间的偏导,从而获得估算的瞬时频率;然后,在对瞬时频率的估算值进行多次迭代的基础上,仅保留时频系数模值最大处所对应的估算瞬时频率,并将其余位置的瞬时频率值归零;最后,对时频系数模值最大处所对应的瞬时频率进行时频重排即可得到细化后的瞬时频带。由于基于MCMSST方法提取的是瞬时频带,故采用时频系数模极大值法在限定的频带范围内提取瞬时频率曲线。通过2组数值算例和1个铝合金悬臂梁质量突变试验,验证了所提方法的有效性。研究结果表明,MCMSST方法不仅彻底解决了未重排点问题,而且提高了瞬时频率的识别精度和抗噪能力。展开更多
基金supported by the National Natural Science Foundation of China(22372001)Starting Fund for Scientific Research of High-Level Talents,Anhui Agricultural University(rc382108)+1 种基金Anhui Provincial Key Research and Development Plan(2022e07020037)Innovation and Entrepreneurship Training Program for College Students(X202310364204,S202210364046,X202310364209)。
文摘Molybdenum carbide(Mo_(2)C)is a promising non-noble metal electrocatalyst with electronic structures similar to Pt for hydrogen evolution reaction(HER).However,strong H^(*)adsorption at the Mo sites hinders the improvement of HER performance.Here,we synthesized monodisperse hollow Mo_(2)C nanoreactors,in which the carbon dots(CD)were in situ formed onto the surface of Mo_(2)C through carburization reactions.According to finite element simulation and analysis,the CD@Mo_(2)C possesses better mesoscale diffusion properties than Mo_(2)C alone.The optimized CD@Mo_(2)C nanoreactor demonstrates superior HER performance in alkaline electrolyte with a low overpotential of 57 mV at 10 mA cm^(−2),which is better than most Mo_(2)C-based electrocatalysts.Moreover,CD@Mo_(2)C exhibits excellent electrochemical stability during 240 h,confirmed by operando Raman and X-ray diffraction(XRD).Density functional theory(DFT)calculations show that carbon dots cause the d-band center of CD@Mo_(2)C to shift away from Fermi level,promoting water dissociation and the desorption of H^(*).This study provides a reasonable strategy towards high-activity Mo-based HER eletrocatalysts by modulating the strength of Mo–H bonds.
文摘针对多重同步挤压变换及其改进算法存在的未重排点问题,提出了一种基于最大系数的多重同步挤压变换(maximum coefficient based multi-synchrosqueezing transform,简称MCMSST)方法来识别时变结构非平稳响应信号的瞬时频率(instantaneous frequency,简称IF)。首先,引入傅里叶频谱来辅助多分量响应信号选取截止频率;其次,对响应信号进行短时傅里叶变换(short time fourier transform,简称STFT),针对短时傅里叶变换系数求取针对时间的偏导,从而获得估算的瞬时频率;然后,在对瞬时频率的估算值进行多次迭代的基础上,仅保留时频系数模值最大处所对应的估算瞬时频率,并将其余位置的瞬时频率值归零;最后,对时频系数模值最大处所对应的瞬时频率进行时频重排即可得到细化后的瞬时频带。由于基于MCMSST方法提取的是瞬时频带,故采用时频系数模极大值法在限定的频带范围内提取瞬时频率曲线。通过2组数值算例和1个铝合金悬臂梁质量突变试验,验证了所提方法的有效性。研究结果表明,MCMSST方法不仅彻底解决了未重排点问题,而且提高了瞬时频率的识别精度和抗噪能力。
