TY - JOUR
T1 - Novel CuCo2O4 Composite Spinel with a Meso-Macroporous Nanosheet Structure for Sulfate Radical Formation and Benzophenone-4 Degradation
T2 - Interface Reaction, Degradation Pathway, and DFT Calculation
AU - Wang, Yiping
AU - Ji, Haodong
AU - Liu, Wen
AU - Xue, Tianshan
AU - Liu, Chao
AU - Zhang, Yuting
AU - Liu, Longyan
AU - Wang, Qiang
AU - Qi, Fei
AU - Xu, Bingbing
AU - Tsang, Daniel C.W.
AU - Chu, Wei
N1 - Funding Information:
This work was performed with the support of the Fundamental Research Funds for the Central Universities (No. 2015ZCQ-HJ-02), the National Natural Science Foundation of China (Nos. 51878047 and 51578520), the Beijing Natural Science Foundation (No. L182027), and the Beijing Forestry University Outstanding Young Talent Cultivation Project (2019JQ03008).
Publisher Copyright:
© 2020 American Chemical Society.
Copyright:
Copyright 2020 Elsevier B.V., All rights reserved.
PY - 2020/5/6
Y1 - 2020/5/6
N2 - A series of CuCo2O4 composite spinels with an interconnected meso-macroporous nanosheet morphology were synthesized using the hydrothermal method and subsequent calcination treatment to activate peroxymonosulfate (PMS) for benzophenone-4 (BP-4) degradation. As-prepared CuCo2O4 composite spinels, especially CuCo-H3 prepared by adding cetyltrimethylammonium bromide, showed superior reactivity for PMS activation. In a typical reaction, BP-4 (10.0 mg/L) was almost completely degraded in 15 min by the activation of PMS (200.0 mg/L) using CuCo-H3 (100.0 mg/L), with only 9.2 μg/L cobalt leaching detected. Even after being used six times, the performance was not influenced by the lower leaching of ions and surface-absorbed intermediates. The possible interface mechanism of PMS activation by CuCo-H3 was proposed, wherein a unique interconnected meso-macroporous nanosheet structure, strong interactions between copper and cobalt, and cycling of Co(II)/Co(III) and Cu(I)/Cu(II) effectively facilitated PMS activation to generate SO4•- and •OH, which contributed to BP-4 degradation. Furthermore, combined with intermediates detected by liquid chromatography quadrupole time-of-flight mass spectrometry and density functional theory calculation results, the degradation pathway of BP-4 involving hydroxylation and C-C bond cleavage was proposed.
AB - A series of CuCo2O4 composite spinels with an interconnected meso-macroporous nanosheet morphology were synthesized using the hydrothermal method and subsequent calcination treatment to activate peroxymonosulfate (PMS) for benzophenone-4 (BP-4) degradation. As-prepared CuCo2O4 composite spinels, especially CuCo-H3 prepared by adding cetyltrimethylammonium bromide, showed superior reactivity for PMS activation. In a typical reaction, BP-4 (10.0 mg/L) was almost completely degraded in 15 min by the activation of PMS (200.0 mg/L) using CuCo-H3 (100.0 mg/L), with only 9.2 μg/L cobalt leaching detected. Even after being used six times, the performance was not influenced by the lower leaching of ions and surface-absorbed intermediates. The possible interface mechanism of PMS activation by CuCo-H3 was proposed, wherein a unique interconnected meso-macroporous nanosheet structure, strong interactions between copper and cobalt, and cycling of Co(II)/Co(III) and Cu(I)/Cu(II) effectively facilitated PMS activation to generate SO4•- and •OH, which contributed to BP-4 degradation. Furthermore, combined with intermediates detected by liquid chromatography quadrupole time-of-flight mass spectrometry and density functional theory calculation results, the degradation pathway of BP-4 involving hydroxylation and C-C bond cleavage was proposed.
KW - CuCo O
KW - benzophenone-4
KW - interconnected meso-macroporous nanosheet
KW - peroxymonosulfate
KW - sulfate radicals
UR - http://www.scopus.com/inward/record.url?scp=85084379958&partnerID=8YFLogxK
U2 - 10.1021/acsami.0c03481
DO - 10.1021/acsami.0c03481
M3 - Journal article
C2 - 32271545
AN - SCOPUS:85084379958
SN - 1944-8244
VL - 12
SP - 20522
EP - 20535
JO - ACS applied materials & interfaces
JF - ACS applied materials & interfaces
IS - 18
ER -