Au@CoS-BiVO4 {010} Constructed for Visible-Light-Assisted Peroxymonosulfate Activation

Au@CoS-BiVO4 {010} Constructed for Visible-Light-Assisted Peroxymonosulfate Activation
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Au@CoS-BiVO4 {010} 构建用于可见光辅助过一硫酸盐活化

DOI:
10.3390/catal11111414
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发表时间:
2021-11-01
期刊:
影响因子:
3.9
通讯作者:
Corvini, Philippe Francois-Xavier
Corvini, Philippe Francois-Xavier
中科院分区:
化学3区
文献类型:
--
作者:
Ji, Yekun;Zhou, Ye;Corvini, Philippe Francois-Xavier

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构建了一个可见光-类Fenton反应体系,用于过一硫酸根选择性转化为硫酸根自由基。当Au@CoS掺杂在单斜BiVO 4 {010}晶面上时,由于m-BiVO 4 {010}和{110}晶面之间的能带不同,促进了空间电荷分离。m-BiVO 4的可见光响应增强,这是由于Au的SPR效应。光生电子通过肖特基结从m-BiVO 4 {010}面转移到Au。由于CoS具有较高的功函数,它能够捕获这些光电子,加速Co(Ⅱ)/Co(Ⅲ)的氧化还原反应,促进过一硫酸根转化为硫酸根自由基(Co2+ + HSO 5 −→ Co 3 + + ·SO 4 − + OH−)。另一方面,空穴在m-BiVO 4 {110}面上的积累也促进了有机物的氧化。因此,超过95%的RhB在40分钟内被降解,并且,即使在五个循环之后,超过80%的RhB可以被去除。自由基捕集实验和EPR证实了硫酸根自由基和光生空穴是有机物降解的主要物种。UV-vis DRS、光致发光(PL)和光电化学分析也证实了可见光响应和电荷分离的增强。在中试规模实验中(PMS = 3 mM,初始TOC = 151 mg/L,反应时间= 4 h),玻璃纤维负载CoS-Au-BiVO 4显示出较高的实际废水矿化率(>60%)。
A visible-light-Fenton-like reaction system was constructed for the selective conversion of peroxymonosulfate to sulfate radical. Au@CoS, when doped on monoclinic BiVO4 {010} facets, promoted spatial charge separation due to the different energy band between the m-BiVO4 {010} and {110} facets. The visible-light response of m-BiVO4 was enhanced, which was attributed to the SPR effect of Au. And the photogenerated electrons were transferred from the m-BiVO4 {010} facet to Au via a Schottky junction. Owing to higher work function, CoS was able to capture these photoelectrons with acceleration of the Co(Ⅱ)/Co(Ⅲ) redox, enhancing peroxymonosulfate conversion to sulfate radical (Co2+ + HSO5−→ Co3+ + •SO4− + OH−). On the other hand, holes accumulated on m-BiVO4 {110} facets also contributed to organics oxidation. Thus, more than 95% of RhB was degraded within 40 min, and, even after five cycles, over 80% of RhB could be removed. The radical trapping experiments and EPR confirmed that both the sulfate radical and photogenerated hole were the main species for organics degradation. UV-vis DRS, photoluminescence (PL) and photoelectrochemical analyses also confirmed the enhancement of the visible-light response and charge separation. In a pilot scale experiment (PMS = 3 mM, initial TOC = 151 mg/L, reaction time = 4 h), CoS-Au-BiVO4 loaded on glass fiber showed a high mineralization rate (>60%) of practical wastewater.