Covalency competition triggers Fe-Co synergistic catalysis for boosted Fenton-like reactions

被引：31

作者：

Li, Wenqian ^{[1
]}

Xia, Shuangqing ^{[1
]}

Wang, Zhenyi ^{[1
]}

Zhang, Bin ^{[1
]}

Li, Boda ^{[1
]}

Zhang, Lijuan ^{[2
,3
]}

Qian, Kun ^{[4
]}

Ma, Jun ^{[1
]}

He, Xu ^{[1
]}

机构：

[1] Harbin Inst Technol, Sch Environm, State Key Lab Urban Water Resource & Environm, Harbin 150090, Peoples R China

[2] Chinese Acad Sci, Key Lab Interfacial Phys & Technol, Shanghai 201800, Peoples R China

[3] Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai Synchrotron Radiat Facil, Shanghai 201204, Peoples R China

[4] Tongji Univ, Coll Environm Sci & Engn, State Key Lab Pollut Control & Resources Reuse, Shanghai 200092, Peoples R China

来源：

APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY | 2023年 / 325卷

基金：

中国国家自然科学基金;

关键词：

Fe-Co synergy; TM-O covalency; PMS activation; Electron transfer; Spinel oxides; HETEROGENEOUS CATALYSTS; AQUEOUS-SOLUTIONS; CHLORINE ATOMS; PEROXYMONOSULFATE; DEGRADATION; ACTIVATION; RADICALS; OXIDE; REDUCTION; MECHANISM;

D O I：

10.1016/j.apcatb.2023.122358

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

Fe-Co based oxides demonstrate excellent Fenton-like catalytic activity, but the intrinsic mechanism of Fe-Co synergy remains elusive. Here, we uncover the influence of covalency competition between Fe and Co on catalytic behaviors in peroxymonosulfate (PMS) activation. Theoretical and experimental analysis reveals that higher electron delocalization of octahedral Co (Co-Oh)-O unit and lower electron delocalization of Fe-Oh-O unit boost electron transfer between Co and O species and transformation of SO5 center dot- towards surface-bounded and free SO4 center dot- instead of O-1(2). With favorable covalency competition, electron transfer capability, active oxidizing species, (Co0.8Fe0.2)(Oh)-O unit exhibits superior activity with rate constant of 0.27 min(-1), 254.7, 37.5 and 2.2 times of that in PMS, Fe-Oh-O unit/PMS and Co-Oh-O unit/PMS systems, respectively, outperforming all the reported Fe-Co based oxides in removal of refractory pollutants. The improved insights into the origin of Fe-Co synergy advance the rational development of highly efficient catalytic oxidation systems for water decontamination.

引用

页数：12

共 54 条

[41] Construction of ternary CuO/CuFe2 O4 /g-C3 N4 composite and its enhanced photocatalytic degradation of tetracycline hydrochloride with persulfate under simulated sunlight [J].

Wang, Lei ;

Ma, Xiaolei ;

Huang, Guofang ;

Lian, Rui ;

Huang, Jingwei ;

She, Houde ;

Wang, Qizhao .

JOURNAL OF ENVIRONMENTAL SCIENCES, 2022, 112 :59-70

[42] Iron-Based Dual Active Site-Mediated Peroxymonosulfate Activation for the Degradation of Emerging Organic Pollutants [J].

Wang, Shizong ;

Xu, Lejin ;

Wang, Jianlong .

ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2021, 55 (22) :15412-15422

[43] Facile synthesis of oxygen vacancies enriched ZnFe2O4 for effective photocatalytic peroxodisulfate activation [J].

Wang, Xinyu ;

Li, Jiajie ;

Chen, Kaiyi ;

Li, Jiajia ;

Jia, Yuefa ;

Mei, Qiong ;

Wang, Qizhao .

SEPARATION AND PURIFICATION TECHNOLOGY, 2022, 303

[44] Ultrahigh Peroxymonosulfate Utilization Efficiency over CuO Nanosheets via Heterogeneous Cu(III) Formation and Preferential Electron Transfer during Degradation of Phenols [J].

Wei, Yan ;

Miao, Jie ;

Ge, Jianxin ;

Lang, Junyu ;

Yu, Chunyang ;

Zhang, Lizhi ;

Alvarez, Pedro J. J. ;

Long, Mingce .

ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2022, 56 (12) :8984-8992

[45] A Strategy to Promote the Electrocatalytic Activity of Spinels for Oxygen Reduction by Structure Reversal [J].

Wu, Guangping ;

Wang, Jun ;

Ding, Wei ;

Nie, Yao ;

Li, Li ;

Qi, Xueqiang ;

Chen, Siguo ;

Wei, Zidong .

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2016, 55 (04) :1340-1344

[46] Analysis of XPS spectra of Fe2+ and Fe3+ ions in oxide materials [J].

Yamashita, Toru ;

Hayes, Peter .

APPLIED SURFACE SCIENCE, 2008, 254 (08) :2441-2449

[47] Iron-cobalt mixed oxide nanocatalysts: Heterogeneous peroxymonosulfate activation, cobalt leaching, and ferromagnetic properties for environmental applications [J].

Yang, Qiujing ;

Choi, Hyeok ;

Al-Abed, Souhail R. ;

Dionysiou, Dionysios D. .

APPLIED CATALYSIS B-ENVIRONMENTAL, 2009, 88 (3-4) :462-469

[48] Spontaneous Delithiation under Operando Condition Triggers Formation of an Amorphous Active Layer in Spinel Cobalt Oxides Electrocatalyst toward Oxygen Evolution [J].

Zhang, Shuo ;

Gu, Songqi ;

Wang, Yu ;

Liang, Chao ;

Yu, Yi ;

Han, Ling ;

Zheng, Shun ;

Zhang, Nian ;

Liu, Xiaosong ;

Zhou, Jing ;

Li, Jiong .

ACS CATALYSIS, 2019, 9 (08) :7389-+

[49] Controlled synthesis of bimetallic Prussian blue analogues to activate peroxymonosulfate for efficient bisphenol A degradation [J].

Zhang, Wuxiang ;

Zhang, Hao ;

Yan, Xin ;

Zhang, Ming ;

Luo, Rui ;

Qi, Junwen ;

Sun, Xiuyun ;

Shen, Jinyou ;

Han, Weiqing ;

Wang, Lianjun ;

Li, Jiansheng .

JOURNAL OF HAZARDOUS MATERIALS, 2020, 387

[50] Application of MOFs and COFs for photocatalysis in CO2 reduction, H2 generation, and environmental treatment [J].

Zhang, Yifeng ;

Liu, Hangxi ;

Gao, Feixue ;

Tan, Xiaoli ;

Cai, Yawen ;

Hu, Baowei ;

Huang, Qifei ;

Fang, Ming ;

Wang, Xiangke .

ENERGYCHEM, 2022, 4 (04)

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