【摘要】 基于不同单金属氧化物对草酸锂（Li₂C₂O₄,LCO）分解的促进效果，以CuO-Mn₂O₃混合物为前驱体，采用简便的固相烧结法合成了一系列Mn、Cu物质的量之比（x）不同的CuMn_xO_1+1.5x双金属氧化物催化剂。通过X射线衍射（XRD）、X射线光电子能谱（XPS）、N₂吸附-脱附等温线和扫描电子显微镜（SEM）等方法表征了材料的结构组成与微观形貌，并探究了其对LCO电化学活性的影响规律。结果表明，在0.05C和2.5～4.5V下，以CuMn_1.1O_2.7为催化剂时LCO的充电比容量可达404.7mAh·g^-1，同时脱锂电位降低至4.44V，首次库仑效率仅为1.3%，可作为正极补锂添加剂应用于磷酸铁锂（LFP）体系；此外，采用密度泛函理论（DFT）计算揭示了LCO分解的速率控制步骤和催化剂的作用机制。将一定量的LCO/CuMn_1.1O_2.7补锂剂添加至LFP浆料中制作成扣式半电池，并对其进行电化学性能测试，结果表明，在最佳补锂剂含量下，相应LFP电极的首次充电比容量为205.9mAh·g^-1,LCO的实际利用率可达74.1%，而且补锂剂的添加能改善LFP的循环性能。更多还原

【Abstract】 In this work,based on the catalytic effect of several metal oxides on the decomposition of lithium oxalate （Li₂C₂O₄,LCO）,a series of CuMnxO_1+1.5xbimetallic oxides with different molar ratios （x） of Mn and Cu were synthe-sized via the controlled calcination of CuO-Mn₂O₃ mixture.The structural composition and surface morphology werecharacterized using the X-ray diffraction （XRD）,X-ray photoelectron spectroscopy （XPS）,N₂ adsorption-desorptionisotherms,and scanning electron microscopy （SEM）.The catalysts were applied in the electrochemical test of LCOat 0.05C within the voltage range of 2.5-4.5 V.Results showed that the charge specific capacity of LCO could beincreased to 404.7 mAh·g^-1and delithium potential can be reduced to 4.44 V with the initial Coulombic efficiencyof 1.3%over CuMn_1.1O_2.7catalyst,which could match with the lithium iron phosphate （LFP） materials as a cathodeprelithiation additive.The rate-determining step of LCO decomposition and the mechanism of the catalyst wererevealed by density functional theory （DFT） calculations.Subsequently,a certain amount of LCO/CuMn_1.1O_2.7wasadded to the LFP slurry,and the corresponding electrochemical performance was tested by assembling half-cells.Itwas found that under the optimal lithium supplement content,the initial charge capacity of the LFP electrode was205.9 mAh·g^-1,and the practical capacity utilization of LCO could reach 74.1%.Moreover,the cycle performanceof LFP can also be improved by using an LCO prelithiation additive.更多还原