Substitutionally Dispersed High-Oxidation CoO_x Clusters in the Lattice of Rutile TiO_2 Triggering Efficient Co-Ti Cooperative Catalytic Centers for Oxygen Evolution Reactions

Yan Yong; Liu Chunyue; Jian Hanwen; Cheng Xing; Hu Ting; Wang Dong; Shang Lu; Chen Ge; Schaaf Peter; Wang Xiayan; Kan Erjun; Zhang Tierui

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Substitutionally Dispersed High-Oxidation CoO_x Clusters in the Lattice of Rutile TiO_2 Triggering Efficient Co-Ti Cooperative Catalytic Centers for Oxygen Evolution Reactions

机译：在金红石TiO_2的晶格中替换高氧化COO_X簇，触发有效的CO-TI合作催化中心进行氧气进化反应

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The development of economical, highly active, and robust electrocatalysts for oxygen evolution reaction (OER) is one of the major obstacles for producing affordable water splitting systems and metal-air batteries. Herein, it is reported that the subnanometric CoOx clusters with high oxidation state substitutionally dispersed in the lattice of rutile TiO2 support (Co-TiO2) can be prepared by a thermally induced phase segregation process. Owing to the strong interaction of CoOx clusters and TiO2 support, Co-TiO2 exhibits both excellent intrinsic activity and durability for OER. The turnover frequency of Co-TiO2 is up to 3.250 s(-1) at overpotentials of 350 mV; this value is one of the highest in terms of OER performance among the current Co-based active materials under similar testing conditions; moreover, the OER current density loss is only 6.5% at a constant overpotential of 400 mV for 30 000 s, which is superior to the benchmark Co3O4 and RuO2 catalysts. Mechanism analysis demonstrates that charge transfer occurs between Co sites and their neighboring Ti atoms, triggering the efficient Co-Ti cooperative catalytic centers, in which OH* and O* are preferred to be adsorbed on the bridging sites of Co and Ti with favorable adsorption energy, inducing a lower energy barrier for O-2 generation.

机译：用于氧气进化反应的经济，高活性和强大的电催化剂的开发是生产经济实惠的水分裂系统和金属电池的主要障碍之一。在此，据报道，具有高氧化态的亚域CoOx簇依赖于金红石TiO 2载体（Co-TiO 2）的晶格（Co-TiO 2），可以通过热诱导的相偏析制备。由于COOO簇和TiO2支持的强相互作用，CO-TiO2表现出优异的内在活动和oer的耐用性。 Co-TiO2的周转频率在350 mV的过电位上高达3.250 s（-1）;该值是在类似测试条件下的当前基于Co-基的活性材料之间的OER性能中最高的。此外，OER电流密度损失在400mV的恒定过电位下仅为6.5％，对于30 000秒，其优于基准CO3O4和RUO2催化剂。机制分析表明，在CO位点和相邻的Ti原子之间发生电荷转移，触发高效的Co-Ti合作催化中心，其中优选在具有良好吸附能量的Co和Ti的桥接位点上吸附在其中的桥接位点，诱导O-2代的较低能量屏障。

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来源
《Advanced Functional Materials》 |2021年第9期|2009610.1-2009610.13|共13页
作者
Yan Yong; Liu Chunyue; Jian Hanwen; Cheng Xing; Hu Ting; Wang Dong; Shang Lu; Chen Ge; Schaaf Peter; Wang Xiayan; Kan Erjun; Zhang Tierui;
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Beijing Univ Technol Ctr Excellence Environm Safety & Biol Effects Dept Chem & Biol Beijing Key Lab Green Catalysis & Separat Beijing 100124 Peoples R China;

Beijing Univ Technol Ctr Excellence Environm Safety & Biol Effects Dept Chem & Biol Beijing Key Lab Green Catalysis & Separat Beijing 100124 Peoples R China;

Nanjing Univ Sci & Technol Inst Energy & Microstruct Dept Appl Phys Nanjing 210094 Peoples R China;

Beijing Univ Technol Fac Environm & Life Sci Beijing Key Lab Green Catalysis & Separat P R China 100124 Peoples R China;

Nanjing Univ Sci & Technol Inst Energy & Microstruct Dept Appl Phys Nanjing 210094 Peoples R China;

TU Ilmenau Inst Mat Sci & Engn Chair Mat Elect Gustav Kirchhoff Str 5 D-98693 Ilmenau Germany|TU Ilmenau Inst Micro & Nanotechnol MarcoNano Gustav Kirchhoff Str 5 D-98693 Ilmenau Germany;

Chinese Acad Sci Tech Inst Phys & Chem Key Lab Photochem Convers & Optoelect Mat Beijing 100190 Peoples R China;

Beijing Univ Technol Fac Environm & Life Sci Beijing Key Lab Green Catalysis & Separat P R China 100124 Peoples R China;

TU Ilmenau Inst Mat Sci & Engn Chair Mat Elect Gustav Kirchhoff Str 5 D-98693 Ilmenau Germany|TU Ilmenau Inst Micro & Nanotechnol MarcoNano Gustav Kirchhoff Str 5 D-98693 Ilmenau Germany;

Beijing Univ Technol Ctr Excellence Environm Safety & Biol Effects Dept Chem & Biol Beijing Key Lab Green Catalysis & Separat Beijing 100124 Peoples R China;

Nanjing Univ Sci & Technol Inst Energy & Microstruct Dept Appl Phys Nanjing 210094 Peoples R China;

Chinese Acad Sci Tech Inst Phys & Chem Key Lab Photochem Convers & Optoelect Mat Beijing 100190 Peoples R China;

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cooperative catalytic centers; CoO; (x) clusters; high oxidation state; oxygen evolution reaction; rutile TiO; (2);

机译：合作催化中心;COO;（x）簇;高氧化态;氧气进化反应;金红石TiO;（2）;

Substitutionally Dispersed High-Oxidation CoO_x Clusters in the Lattice of Rutile TiO_2 Triggering Efficient Co-Ti Cooperative Catalytic Centers for Oxygen Evolution Reactions

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