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酞菁铁(FePc)分子催化剂

作者:互联网

酞菁铁(FePc)分子催化剂

在已知的非Pt-ORR催化剂中,酞菁铁(FePc)分子催化剂因其独特的FeN4活性中心和较低的反应能垒而备受关注。然而,具有平面对称FeN4位点的FePc由于其对O2的吸附和活化能力较差,通常表现出较差的ORR活性。因此,打破电子结构的对称性将是提高FePc催化剂对O2的吸附/活化从而大大提高其ORR活性的有效策略。

要点一:理论计算表明,Fe-O配位引起O-FeN4位轴向的电子局域化,从而增强O2的吸附和活化。

 

a. 分子结构模型。

b. FeAB-O和FePc/AB的电子局域化函数。

c. FeAB-O和FePc/AB的Bader电荷转移和O2吸附能。

d. FeAB-O和FePc/AB上ORR路径的自由能图。

要点二:将FePc与氧功能化的碳配位,利用同步辐射X射线吸收和穆斯堡尔谱表征FePc与碳的Fe-O配位。

 

a. 原始FeAB-O,FePc/AB,AB,AB-O和FePc的XRD图谱。

b. FeAB-O和FePc/AB的XPS Fe2p谱。

c. FeAB-O,FePc/AB,Fe和Fe2O3的Fe K-edge X射线近边吸收谱。

d. FeAB–O、FePc/AB和Fe2O3中Fe K edge的扩展X射线吸收精细结构(EXAFS)光谱。

 

a. 57Fe穆斯堡尔透射光谱。

b. 氧气吸附-脱附试验。

c. 大气中的TGA曲线。

d. FeAB-O和FePc/AB的O2-TPD曲线。

要点三:所得催化剂对O2的吸附和活化动力学较快,Tafel斜率为27.5 mV dec-1,半波电位为0.90 V。

FeAB-O在N2饱和和O2溶解的0.1M KOH溶液中的循环伏安曲线。

b. FeAB-O,FePc/AB,Pt/C在饱和0.1 M KOH中的极化曲线。

c. FeAB–O、FePc/AB和Pt/c在0.88 V下的半波电位和Jk值。

d. FeAB–O、FePc/AB和Pt/C对应的Tafel图。

e. FeAB–O和Pt/C中电子转移数和生成H2O2的比例。

f. FeAB–O和Pt/C的 I–t计时电流响应(O2饱和0.1 M KOH,转速1600 rpm)。

通过在O2等离子体处理的乙炔黑(AB-O)基体上,将FePc分子与含氧基团进行配位设计了一种复合催化剂(FeAB-O),实现了对O2的有效吸附和活化。理论计算表明,轴向O配位(O-FeN4)破坏了Fe的电子分布对称性,导致O上的电子局域化,O-FeN4位点上明显的电子局域化有利于O2的轴向吸附和活化。

X射线吸附实验和O2吸附/解吸实验分别证实了FeAB-O催化剂的轴向O配位和优异的O2吸附能力。ORR性能测试表明,优化后的FeAB–O催化剂具有27.5 mV dec−1的超低Tafel斜率和0.90 V的半波电位,比而无轴向O配位的Fe/AB高30mV,比Pt/C高50 mV。

产品名称别名英文名称cas

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二氰基吡嗪类&类似物 [酞菁砌块]

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1,4,5,6-四氢-5,6-二氧-2,3-二氰基吡嗪1,4,5,6-四氢-5,6-二氧-2,3-吡嗪二甲腈1,4,5,6-Tetrahydro-5,6-dioxo-2,3-pyrazinedicarbonitrile36023-64-0

5,6-二氨基-2,3-二氰基吡嗪2,3-二氰基-5,6-二氨基吡嗪5,6-Diamino-2,3-dicyanopyrazine36023-58-2

2,3-二氰基-5-甲基吡嗪5-Methyl-2,3-pyrazinedicarbonitrile2,3-Dicyano-5-methylpyrazine52197-12-3

吡啶-2,3-二甲腈2,3-二氰基吡啶Pyridine-2,3-dicarbonitrile17132-78-4

2,3-二氰基吡嗪吡嗪-2,3-二甲腈2,3-Dicyanopyrazine13481-25-9

4,5-二氰基咪唑DCI/4,5-二氰咪唑4,5-Dicyanoimidazole1122-28-7

5,6-二氯-2,3-二氰基吡嗪5,6-Dichloro-2,3-pyrazinedicarbonitrile5,6-Dichloro-2,3-dicyanopyrazine56413-95-7

2,3-二氰基-5-氨基-6-氯吡嗪5-氨基-6-氯-2,3-二氰基吡嗪5-Amino-6-chloro-2,3-dicyanopyrazine56413-96-8

邻苯二甲腈类 [酞菁砌块]

4-硝基邻苯二甲腈1,2-二氰基-4-硝基苯4-Nitrophthalonitrile31643-49-9

1,3-二亚氨基异吲哚啉1,3-Diiminoisoindoline57500-34-2

4-碘酞腈1,2-二氰基-4-碘苯4-Iodophthalonitrile69518-17-8

3-硝基邻苯二甲腈1,2-二氰基-3-硝基苯3-Nitrophthalonitrile51762-67-5

4-(4-α-异丙苯基苯氧基)苯二甲腈2-[4-(3,4-Dicyanophenoxy)phenyl]-2-phenylpropane4-(4-α-Cumylphenoxy)phthalonitrile83482-57-9

4-戊氧基苯二甲腈4-戊氧基邻苯二甲腈4-Pentyloxyphthalonitrile106943-83-3

4-溴邻苯二甲腈4-溴-1,2-二氰基苯4-Bromophthalonitrile70484-01-4

4-正丁氧基-1,2-二氰苯4-丁氧基邻苯二甲腈4-Butoxyphthalonitrile81560-32-9

4-己氧基苯二甲腈1,2-Dicyano-4-hexyloxybenzene4-Hexyloxyphthalonitrile104949-82-8

4-丙氧基邻苯二甲腈4-丙氧基苯二甲腈4-Propoxyphthalonitrile106144-18-7

4-氨基邻苯二甲腈3,4-二氰基苯胺4-Aminophthalonitrile56765-79-8

1,2-二氰基-4-氟苯4-氟邻苯二腈4-Fluorophthalonitrile65610-14-2

4,5-二氟酞腈1,2-二氰基-4,5-二氟苯4,5-Difluorophthalonitrile134450-56-9

4,5-二氨基酞腈1,2-二氨基-4,5-二氰基苯4,5-Diaminophthalonitrile129365-93-1

4-(2',6'-二甲基苯氧基)邻苯二甲腈1,2-二氰基-4-(2',6'-二甲基苯氧基)苯4-(2',6'-Dimethylphenoxy)phthalonitrile221302-75-6

4,5-二氯邻苯二甲腈1,2-二氯-4,5-二氰基苯4,5-Dichlorophthalonitrile139152-08-2

邻苯二甲腈1,2-二氰基苯Phthalonitrile91-15-6

全氯邻苯二甲腈四氯邻苯二甲腈Tetrachlorophthalonitrile1953-99-7

4-叔丁基邻苯二甲腈4-叔丁基-1,2-二氰基苯4-tert-Butylphthalonitrile32703-80-3

四氟邻苯二甲腈3,4,5,6-四氟邻苯二甲腈Tetrafluorophthalonitrile1835-65-0

4-羟基邻苯二甲腈3,4-二氰基苯酚4-Hydroxyphthalonitrile30757-50-7

1,2-Dicyano-4-dodecyloxybenzene4-十二烷氧基邻苯二甲腈4-Dodecyloxyphthalonitrile161082-75-3

1,2,4,5-四氰基苯1,2,4,5-苯四甲腈1,2,4,5-Tetracyanobenzene712-74-3

2,3-二氰基对苯二酚3,6-二羟基邻苯二甲腈

2,3-二氰基羟基醌

3,6-二羟基邻苯二腈

3,6-二羟基邻苯二甲氰

2,3-二氰基氢醌

2,3-Dicyanohydroquinone4733-50-0

萘二甲腈类 [酞菁砌块]

1,2-萘二甲腈1,2-二氰基萘1,2-Naphthalenedicarbonitrile19291-76-0

1,3-二亚氨基苯并[f]异吲哚啉1,3-Diiminobenz[f]isoindoline65558-69-2

2,3-二氰基-6-硝基萘2,3-Dicyano-6-nitronaphthalene184026-06-0

2,3-二溴-6,7-二氰基萘6,7-Dibromonaphthalene-2,3-dicarbonitrile2,3-Dibromo-6,7-dicyanonaphthalene74815-81-9

2,3-二氰基-1,4-二羟基-5-硝基萘2,3-二氰基-5-硝基-1,4-萘二醇2,3-Dicyano-1,4-dihydroxy-5-nitronaphthalene4655-62-3

6-溴-2,3-二氰基萘6-溴萘-2,3-二甲腈6-Bromo-2,3-dicyanonaphthalene70484-02-5

2,3-二氰基萘2,3-萘二甲腈2,3-Dicyanonaphthalene22856-30-0

wyf  01.04

标签:10,20,15,II,苯基,催化剂,FePc,酞菁
来源: https://blog.csdn.net/zhaocaijinbaoya/article/details/112195267