Synthesis and characterization of titanium oxynitride catalyst via direct ammonia nitridation of titanium polyacrylate for oxygen reduction reaction

IF 3.4 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY International Journal of Mechanical and Materials Engineering Pub Date : 2024-11-18 DOI:10.1186/s40712-024-00189-1
Yushi Tamaki, Satoshi Seino, Naoki Shinyoshi, Yuta Uetake, Takaaki Nagai, Ryuji Monden, Akimitsu Ishihara, Takashi Nakagawa
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Abstract

A titanium oxynitride catalyst for the oxygen reduction reaction (ORR) in polymer electrolyte fuel cells was synthesized through the direct ammonia nitridation of titanium complexes. Titanium polyacrylate was employed as the catalyst precursor, and the effect of the calcination temperature between 600 and 1000 °C on the catalyst structure was studied. The catalysts were characterized via X-ray diffraction, X-ray absorption spectroscopy, transmission electron microscopy, cyclic voltammetry, and powder electrical resistivity measurements. The formation of titanium oxynitride particles and deposited carbon was observed for all the samples; however, significant variations in the catalyst structure and catalytic activity were also observed. With an increase in the calcination temperature, nitridation of titanium oxynitride progressed, and the conductivity of the catalyst powder increased. The highest rest potential and ORR current density were achieved with calcination at 800 °C. Importantly, the results suggest that maintaining an optimal nitrogen doping level within the catalyst particles, along with ensuring the formation of electroconductive deposited carbon, is essential for achieving a high ORR current. This work introduces the direct ammonia nitridation of metal complexes as a promising process for designing metal oxynitride catalysts.

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通过氨氮直接氮化聚丙烯酸钛制备用于氧还原反应的氮化钛催化剂的合成与表征
通过氨直接氮化钛络合物,合成了一种用于聚合物电解质燃料电池中氧还原反应(ORR)的氮化钛催化剂。采用聚丙烯酸钛作为催化剂前驱体,并研究了 600 至 1000 °C 煅烧温度对催化剂结构的影响。通过 X 射线衍射、X 射线吸收光谱、透射电子显微镜、循环伏安法和粉末电阻率测量对催化剂进行了表征。所有样品都观察到了氧化钛颗粒和沉积碳的形成,但催化剂结构和催化活性也有显著差异。随着煅烧温度的升高,氧化氮钛的氮化作用逐渐增强,催化剂粉末的电导率也随之升高。在 800 °C 煅烧时,静电电位和 ORR 电流密度最高。重要的是,研究结果表明,保持催化剂颗粒内最佳的氮掺杂水平,同时确保形成导电沉积碳,是获得高 ORR 电流的关键。这项研究将金属复合物的直接氨氮化作为设计金属氮氧化物催化剂的一种有前途的工艺。
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CiteScore
8.60
自引率
0.00%
发文量
1
审稿时长
13 weeks
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