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Cobalt Single Atoms on Tetrapyridomacrocyclic Support for Efficient Peroxymonosulfate Activation
Environmental Science & Technology ( IF 10.8 ) Pub Date : 2020-11-19 , DOI: 10.1021/acs.est.0c06086 Chiheng Chu 1, 2 , Ji Yang 3 , Xuechen Zhou 2 , Dahong Huang 2 , Haifeng Qi , Seunghyun Weon 2 , Jianfeng Li 3 , Menachem Elimelech 2 , Aiqin Wang , Jae-Hong Kim 2
Environmental Science & Technology ( IF 10.8 ) Pub Date : 2020-11-19 , DOI: 10.1021/acs.est.0c06086 Chiheng Chu 1, 2 , Ji Yang 3 , Xuechen Zhou 2 , Dahong Huang 2 , Haifeng Qi , Seunghyun Weon 2 , Jianfeng Li 3 , Menachem Elimelech 2 , Aiqin Wang , Jae-Hong Kim 2
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Transition-metal catalysts that can efficiently activate peroxide bonds have been extensively pursued for various applications including environmental remediation, chemical synthesis, and sensing. Here, we present pyridine-coordinated Co single atoms embedded in a polyaromatic macrostructure as a highly efficient peroxide-activation catalyst. The efficient catalytic production of reactive radicals through peroxymonosulfate activation was demonstrated by the rapid removal of model aqueous pollutants of environmental and public health concerns such as bisphenol A, without pH limitation and Co2+ leaching. The turnover frequency of the newly synthesized Co single-atom catalyst bound to tetrapyridomacrocyclic ligands was found to be 2 to 4 orders of magnitude greater than that of benchmark homogeneous (Co2+) and nanoparticulate (Co3O4) catalysts. Experimental results and density functional theory simulation suggest that the abundant π-conjugation in the polyaromatic support and strong metal–support electronic interaction allow the catalysts to effectively adsorb and activate the peroxide precursor. We further loaded the catalysts onto a widely used poly(vinylidene fluoride) microfiltration membrane and demonstrated that the model pollutants were oxidatively removed as they simply passed through the filter, suggesting the promise of utilizing this novel catalyst for realistic applications.
中文翻译：
四环大环支持高效过氧单硫酸盐活化钴单原子。
可以有效活化过氧化物键的过渡金属催化剂已广泛用于各种应用，包括环境修复，化学合成和传感。在这里，我们介绍嵌入吡啶在多芳香族宏观结构中作为高效过氧化物活化催化剂的钴配位的单原子。通过快速去除环境和公共卫生问题的模型水性污染物（如双酚A）而不受pH限制和Co 2+浸出的影响，证明了通过过氧一硫酸盐活化可有效催化生产自由基。发现与四吡啶并大环配体结合的新合成的Co单原子催化剂的周转频率比基准均相（Co2+）和纳米颗粒（Co 3 O 4）催化剂。实验结果和密度泛函理论模拟表明，聚芳烃载体中大量的π共轭和强金属与载体的电子相互作用使催化剂能够有效地吸附和活化过氧化物前体。我们进一步将催化剂加载到广泛使用的聚偏二氟乙烯微滤膜上，并证明模型污染物仅通过过滤器就被氧化去除，这表明将这种新型催化剂用于实际应用的希望。
更新日期：2021-01-19
中文翻译：
四环大环支持高效过氧单硫酸盐活化钴单原子。
可以有效活化过氧化物键的过渡金属催化剂已广泛用于各种应用，包括环境修复，化学合成和传感。在这里，我们介绍嵌入吡啶在多芳香族宏观结构中作为高效过氧化物活化催化剂的钴配位的单原子。通过快速去除环境和公共卫生问题的模型水性污染物（如双酚A）而不受pH限制和Co 2+浸出的影响，证明了通过过氧一硫酸盐活化可有效催化生产自由基。发现与四吡啶并大环配体结合的新合成的Co单原子催化剂的周转频率比基准均相（Co2+）和纳米颗粒（Co 3 O 4）催化剂。实验结果和密度泛函理论模拟表明，聚芳烃载体中大量的π共轭和强金属与载体的电子相互作用使催化剂能够有效地吸附和活化过氧化物前体。我们进一步将催化剂加载到广泛使用的聚偏二氟乙烯微滤膜上，并证明模型污染物仅通过过滤器就被氧化去除，这表明将这种新型催化剂用于实际应用的希望。
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