Tuning of ORR activity through the stabilization of the adsorbates by hydrogen bonding with substituent groups
文献信息
Nagaprasad Reddy Samala, Ilya Grinberg
Metallocorroles and metalloporphyrins (M–N–C) are some of the best alternative molecular catalysts for the replacement of the expensive platinum-group metals (PGM) in oxygen reduction reaction (ORR) catalysis in polymer electrolyte membrane (PEM) fuel cells. To date, Co-based corroles have shown the best performance, but still suffer from the poor stability and the toxicity of the Co metal. Mn–N–C are more stable than Co–N–C, and are also less reactive towards peroxide formation. In this work, using first-principles density functional theory calculations, we study the improvement of the Mn-based corrole ORR activity by exploiting hydrogen bonding with substituent groups to modify the adsorption energies of the ORR intermediates and obtain higher onset potential (Vonset) values. We found that by using phenyl acetic acid as a substituent, Vonset increased from 0.54 V for the unsubstituted corrole to ∼0.9 V which is competitive with the Vonset of the Co-based corroles. Our results suggest that hydrogen bonding with substituent groups should be considered in the analysis and design of the reactivity of active sites in non-PGM ORR catalysts.
相关文献
Dependence of hot electron transfer on surface coverage and adsorbate species at semiconductor–molecule interfaces
Lesheng Li, Yosuke Kanai
DOI: 10.1039/C7CP07247C
Defect evolution in ZnO and its effect on radiation tolerance
Jinpeng Lv, Xingji Li
DOI: 10.1039/C8CP01855C
Excimer formation and evolution of excited state properties in discrete dimeric stacking of an anthracene derivative: a computational investigation
Yu Gao, Haichao Liu, Shitong Zhang, Qiang Gu, Yue Shen, Yunpeng Ge, Bing Yang
DOI: 10.1039/C8CP00834E
The fate of plasma-generated oxygen atoms in aqueous solutions: non-equilibrium atmospheric pressure plasmas as an efficient source of atomic O(aq)
J. Benedikt, A. Shaw, B. R. Buckley, F. Iza, S. Schäkermann, J. E. Bandow
DOI: 10.1039/C8CP00197A
How changes in interfacial pH lead to new voltammetric features: the case of the electrochemical oxidation of hydrazine
Antony Cyril Arulrajan, Christophe Renault, Stanley C. S. Lai
DOI: 10.1039/C8CP01835A
Electron-stimulated reactions in nanoscale water films adsorbed on α-Al2O3(0001)
Nikolay G. Petrik, Greg A. Kimmel
DOI: 10.1039/C8CP01284A
Quantum anomalous/valley Hall effect and tunable quantum state in hydrogenated arsenene decorated with a transition metal
Jian-Zhou Zhao, Cui-E Hu, Xiang-Rong Chen, Xiao-Lin Zhou
DOI: 10.1039/C8CP00005K
A sinter-resistant catalyst using an alumina support recycled from AlP fumigation residue: trash to treasure
Jinshi Dong, Jun Wang, Jianqiang Wang, Guanghao Cheng, Tianming Huang
DOI: 10.1039/C8CP00111A
Rationalisation of the optical signatures of nor-dihydroxanthene-hemicyanine fused near-infrared fluorophores by first-principle tools
Cloé Azarias, Isabelle Navizet, Paul Fleurat-Lessard, Boris Le Guennic, Jean-Alexandre Richard, Denis Jacquemin
DOI: 10.1039/C8CP01587B
您可能还喜欢
3 - (二氟甲基)-1 -氟苯(CAS号:26029-52-7)适用哪些法规指南?
3 - (二氟甲基)-1 -氟苯需遵循联合国全球化学品统一分类和标签制度(GHS),包括急性毒性、皮肤腐蚀/刺激、严重眼损伤/眼刺激等分类。同时,该化合物还需符...
3,5-二甲基苯胺(CAS号:108-69-0)通常如何合成?
3,5-二甲基苯胺通常通过乙苯的氨解反应合成。反应中使用硫酸作为催化剂,反应温度为120-130°C。乙苯在硫酸存在下与氨反应,生成3,5-二甲基苯胺和苯胺副产...
3-甲基异噻唑-5-胺(CAS号:24340-76-9)安全吗?
3-甲基异噻唑-5-胺在适当使用和储存条件下是相对安全的,但在操作时应注意防护措施。应避免吸入粉尘,避免与皮肤和眼睛直接接触。在操作过程中,应穿戴适当的防护装备...
3-(1,3-Thiazol-2-yl)-1H-indole(CAS号:135531-86-1)通常如何合成?
3-(1,3-噻唑-2-基)-1H-吲哚通常通过多步合成方法制备。首先,由噻唑-2-基溴化物和吲哚进行偶联反应,得到中间体。然后,通过还原反应将中间体转化为所需...
4-溴-2-氟苯甲基氯(CAS号:85510-82-3)的主要用途是什么?
4-溴-2-氟苯甲基氯主要用于有机合成中间体,特别是在医药、农药和染料等领域。作为一种具有特定结构的化合物,它在合成复杂有机分子时扮演重要角色。
处理Fmoc-β-(3-噻吩基)-D-Ala-OH(CAS号:220497-90-5)时应注意哪些实验室安全事项?
处理Fmoc-β-(3-噻吩基)-D-Ala-OH时,应佩戴防护手套、护目镜和实验服。操作应在通风橱内进行。如发生泄露,应立即用大量水冲洗,并通知实验室管理人员...
氮化硅(CAS号:12033-89-5)通常如何合成?
氮化硅通常通过氮化硅的直接反应合成,即在高温下将四氯化硅与氨气反应。具体步骤是将四氯化硅和氨气混合并加热至1300-1700℃,在该条件下,四氯化硅与氨气反应生...
Cetirizine EP Impurity B DiHCl(CAS号:1000690-91-4)通常如何合成?
Cetirizine EP Impurity B DiHCl通常通过一锅法合成,首先将4-氯苯基-苯甲基氯甲酸酯与1-哌嗪乙酸反应,生成相应的酸,然后与盐酸反应...
如何储存1-哌啶-4-基丁-1-酮(CAS号:3509-15-7)?
1-哌啶-4-基丁-1-酮应储存在阴凉、干燥的地方,避免阳光直射。存储容器应密封,并确保通风良好。建议储存温度不超过25℃,湿度保持在相对较低的水平。
如何处理含有VORUCICLIB(CAS号:1000023-04-0)的废料?
含有VORUCICLIB的废料应进行专业的收集和处理,包括使用适当的容器进行隔离,避免与其他化学品接触。处理方法通常包括化学中和、沉淀反应或吸附过程,随后进行焚...
来源期刊
Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.










![Methyl 4-({[(2-methyl-2-propanyl)oxy]carbonyl}amino)bicyclo[2.2.2]octane-1-carboxylate structure Methyl 4-({[(2-methyl-2-propanyl)oxy]carbonyl}amino)bicyclo[2.2.2]octane-1-carboxylate structure](https://cnstatic.chemtradehub.com/structs/943/943845-74-7-b7e5.webp)


![4-Chloro-3-(trifluoromethyl)-1H-pyrrolo[2,3-b]pyridine structure 4-Chloro-3-(trifluoromethyl)-1H-pyrrolo[2,3-b]pyridine structure](https://cnstatic.chemtradehub.com/structs/869/869335-75-1-a9d0.webp)
