Journal of Materials Chemistry A
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2022
·Vol. 10
·期 10
·5430-5441
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IF 14.511
Huaijie Shi,Ge Feng,Suiqin Li,Jia Liu,Xinying Yang,Ye Li,Ye Lu,Xing Zhong,Shibin Wang,Jianguo Wang
An alternative method for producing ozone, electrochemical ozone production (EOP) is a major area of interest in the field of in situ sterilization and disinfection. However, commercial lead dioxide as a traditional anodic electrocatalyst is highly toxic and has low durability, and exploring anodic electrocatalysts with lower lead content and performance loss is challenging. Herein, a series of pyramidal sillenite-type Bi12PbO20 materials were designed and fabricated with a hydrothermal method in which Pb was introduced to Bi2O3 frameworks. The product, Bi12PbO20-3, exhibited remarkable EOP performance, with faradaic efficiency of 15.1% at 50 mA cm−2 in a neutral solution, which was almost 1.5 times that of commercial β-PbO2. Computational simulations further demonstrated that the confined [Pb–O4] fragment was confined in the Bi–O bonding environment of Bi12PbO20, the low oxygen vacancy formation energy resulted from the weak Pb–O interaction and remarkably enhanced EOP activity. Such a local confined environment plays a vital role in suppressing Pb loss, thereby accounting for the robust EOP stability. Additionally, the significant performance of the membrane electrode assembly system in the electrochemical degradation of antibiotics and pesticides implied the potential environmental application capabilities of Bi12PbO20.
研究领域:
材料科学
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环境科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2025
·
IF 4.3
Fengying Gao,Xinyu Li,Lihao Liu,Mengmeng Lu,Huaijie Shi,Xuan Yu,Lei Ding,Shibin Wang,Sheng Dai,Xing Zhong,Jianguo Wang
Platinum-based electrocatalysts exhibited good performance in electrocatalytic ozone production (EOP) and hydrogen evolution reaction (HER). Nonetheless, the widespread application of platinum is restricted due to its limited availability and high cost. In this study, we propose an alloying strategy for the synthesis of PtCo/Co 2 B, which achieved a Faraday efficiency (FE) of 9.09 % for EOP and overpotential of 51.5 mV for HER at 10 mA⋅cm −2 in acidic conditions. Theoretical calculations demonstrate that the synergy between the PtCo and Co 2 B in PtCo/Co 2 B modulates the adsorption properties of the O 3 * intermediate, thereby facilitating the reaction towards the EOP. Furthermore, the chemisorption energy of hydrogen is approximately zero, indicating optimal electrocatalytic activity for HER. Such unique structure enhances the performance of electrocatalyst and significantly extends its durability in practical applications. In addition to its electrochemical performance, the PtCo/Co 2 B electrocatalyst effectively degrades organic pollutants and demonstrates strong sterilization capabilities.
研究领域:
材料科学
·
电化学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Energy Chemistry
·
2025
·
IF 14.9
Zhaoyu Chen,Ben Zhang,Shuyan Lu,Guanfeng Xue,Qianzhi Gou,Jiacheng Wang,Ruduan Yuan,Juanxiu Xiao,Li Li,John Wang,Meng Li
Electrochemical ozone (O 3 ) production (EOP) faces a critical challenge due to the competitive oxygen evolution reaction (OER), which severely limits ozone yields. Inspired by the oxygen-binding mechanism of heme, we designed a biomimetic catalyst, FePP@SnO 2 @CA, by electrodepositing iron porphyrin (FePP) onto SnO 2 @CA nanosheets, endowing it with an “oxygen-locking property” to suppress competing OER. This catalyst demonstrates exceptional EOP performance, achieving an ozone production rate of 8.9 mmol cm −2 h −1 and a Faraday efficiency (FE) of 20.46% ± 1.6%. DFT calculations confirm that Fe–O 2 interactions stabilize O 2 * intermediates, redirecting the reaction pathway from OER to ozone generation and reducing the O–O coupling energy barrier, thereby enabling thermodynamic selectivity control. In addition, when FePP@SnO 2 @CA is used as a dual-functional material for sea sand desalination, the chlorine removal efficiency can reach 52.7%. This work provides a novel bioinspired strategy for EOP catalyst design and broadens the application potential of FePP@SnO 2 @CA in sustainable technologies.
研究领域:
材料科学
·
环境科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
ELECTROCHIMICA ACTA
·
2024
·
IF 5.5
Shao-Kang Deng,Jin-Tao Jiang,Tsung-Lin Tsai,Xin-Hua Xu,Li-Hua Cheng
The crystal facet of PbO 2 has been proved to be a key factor affecting its electrochemical ozone production (EOP) performance. However, PbO 2 with smooth and uniform crystal surface and single-crystal nature, which is the basis and prerequisite for PbO 2 crystal facet engineering, has not yet been reported. In this study, by adding polyvinylpyrrolidone (PVP) as a facet modifier during the hydrothermal synthesis, a quasi-single-crystal PbO 2 (PVP:Pb(CH 3 COO) 2 ·3H 2 O=48:100, PVP-48) with (110) and (101) exposed facets was successfully synthesized. Compared with commercial PbO 2 prepared by electrochemical deposition, PVP-48 exhibits excellent electrochemical catalytic activity due to its special crystal structure, and achieves the highest current efficiency of 11.9 % at a current density of 0.83 A/cm 2 . Further calculations show that PVP prefers to adsorb onto the (110) facet of the lead dioxide and reduces its surface energy, thereby exposing the (110) facet more readily. This work demonstrates the importance of PbO 2 facets composition and provides new ideas for further controllable synthesis of PbO 2 with specific facet structure and higher EOP efficiency.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2024
·
IF 15.7
Jia Liu,Shibin Wang,Jinfu Cai,Lizhen Wu,Yun Liu,Jiahui He,Zaixiang Xu,Xiaoge Peng,Xing Zhong,Liang An,Jianguo Wang
Electrochemical ozone production (EOP) is an intrinsically safe technology compared to Corona discharge methods for ozone generation. However, EOP technology exhibits higher electrical utility demand. Herein, a square-shaped lead oxide (PbO x -CTAB-120) electrocatalyst with outstanding EOP activity has been successfully prepared by a simple method. Then the PbO x -CTAB-120 was assembled into a newly visualized EOP electrolyzer (with parallel flow field) at 1.0 A cm −2 in ultrapure water. The gaseous ozone yield reached 588 mg h −1 g −1 catalyst , corresponding to a specific energy consumption (P EOP ) of 56 Wh g −1 gaseous ozone . In-situ 18 O isotope-labelled differential electrochemical mass spectrometry reveals that PbO x -CTAB-120 undergoes phase shuttling to β-PbO 2 via the lattice oxygen oxidation mechanism pathway. Furthermore, density functional theory calculations for multiple reaction pathways on the Pb 3 O 4 (110) surface also demonstrated the participance of lattice oxygen in the EOP process, with the results show that the oxygen vacancy generated from lattice oxygen migration could effectively stabilize the OOH* and O 2 * reaction intermediate in contrast to the adsorbate evolution mechanism. Therefore, the presence of highly stabilized surfaces Pb 3 O 4 (110) on PbO x -CTAB-120 before phase shuttling and the stabilization of β-PbO 2 (101) and β-PbO 2 (110) crystalline surfaces after phase shuttling allowed PbO x -CTAB-120 to maintain its excellent EOP activity and stability. Moreover, based on computational fluid dynamics simulations and experimental observations, the parallel flow field design facilitated efficient mass transfer of the gaseous product (O 2 +O 3 ) and effective thermal dissipation of the system. In addition, the high activity electrocatalyst coupled with the optimized EOP electrolyzer enabled efficient in-situ degradation of organic species.
研究领域:
电化学
·
催化
·
环境科学
·
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）