Frontiers in Energy Research
·
2021
·
IF 4.008
Li Jiayi,Zhou Wei,Huang Yuming,Gao Jihui
Replacing the oxygen evolution reaction (OER), which is of high energy consumption and slow kinetics, with the more thermodynamically favorable reaction at the anode can reduce the electricity consumption for hydrogen production. Here we developed a lignin-assisted water electrolysis (LAWE) process by using Ti/PbO2 with high OER overpotential as the anode aimed at decreasing the energy consumption for hydrogen production. The influence of key operating parameters such as temperature and lignin concentration on hydrogen production was analyzed. Compared with alkaline water electrolysis (AWE), the anode potential can be decreased from 0.773 to 0.303 (V vs. Hg/HgO) at 10 mA/cm2 in LAWE, and the corresponding cell voltage can be reduced by 546 mV. With increasing the temperature and lignin concentration, current density and H2 production rate were efficiently promoted. Furthermore, the anode deactivation was investigated by analyzing the linear sweep voltammetry (LSV) and cyclic voltammetry (CV) tests. Results showed that the anode deactivation was affected by the temperature.
研究领域:
能源化学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
RSC Advances
·
2018
·Vol. 8
·期 12
·6206-6211
·
IF 2.936
Tong Qi,Ziqi Su,Yan Jin,Yuqing Ge,Hui Guo,Hui Zhao,Jiaqiang Xu,Qinghui Jin,Jianlong Zhao
Total phosphorus is one of the key water quality parameters in environmental monitoring. To precisely determine the total phosphorus, water samples have to be pretreated to convert the various forms of phosphorus to orthophosphate. Conventionally, pretreatment is accomplished by heating, acidification, and oxidation in a digestion equipment, which is dangerous, time-consuming, and complicated. Herein, we propose a novel high-performance electrochemical oxidation protocol for phosphorus digestion based on a PbO2 electrode. The electrode, which has a hydrophobic and stable surface, was prepared by electrochemical deposition on a titanium substrate and has high hydroxyl radical utilization when digesting total phosphorus. As a result, 90% of sodium glycerophosphate was digested within 30 minutes, and high digestion ratios of acephate, glyphosate, and inland water samples were obtained as well. In addition, this electrochemical digestion protocol does not required heating and acidification steps, which shortens the digestion time. Therefore, a rapid quantification of total phosphorus in the water sample was achieved.
研究领域:
环境科学
·
分析化学
✓ 已验证
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2015
·
IF 4.321
Qizhou Dai,Jiazhong Zhou,Xiaoyang Meng,Daolun Feng,Chengqiang Wu,Jianmeng Chen
A novel molybdenum modified PbO 2 electrode was successfully prepared with the method of electrodeposition . The SEM and XRD were employed to study the surface morphology of electrodes, which indicated that the modified PbO 2 electrode had a larger effective area and more compact film. Electrochemical degradation of cinnamic acid (CA) in aqueous solution with Mo–PbO 2 electrode and PbO 2 electrode were investigated. The results showed that the Mo–PbO 2 electrode had a better effect of CA removal. The operational parameters influencing the electrochemical degradation of CA with Mo–PbO 2 electrode were optimized and the results revealed that the electrochemical degradation of CA followed the pseudo-first-order kinetics and the optimal removal of CA and COD were 85.51% and 25.79% after 120 min on condition of the electrolyte concentration, initial concentration of CA, current density and initial value of pH were 0.1 mol/L, 300 mg/L, 10 mA/cm 2 and 3.4, respectively. The degradation mechanism of CA in electrochemical oxidation with Mo–PbO 2 electrode was analyzed and the main degradation pathway of CA was proposed based on the intermediates identified by IC and GC–MS.
研究领域:
环境科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2022
·
IF 14.224
Shuaishuai Man,Dehui Luo,Qing Sun,Haifeng Yang,Hebin Bao,Ke Xu,Xuzhong Zeng,Miao He,Zehao Yin,Li Wang,Zhihong Mo,Wenjing Yang,Xueming Li
Stable electrode materials with high catalytic activity are urgently required for electrochemical degradation of refractory organic pollutants in wastewater treatment . Herein, high conductive MXene (Ti 3 C 2 T x ) was firstly fabricated by electrophoretic deposition (EPD) as an interlayer for preparing a novel PbO 2 electrode. The well-conducted Ti 3 C 2 T x interlayer significantly improved the electrochemical performance of the EPD-2.0/PbO 2 (EPD time was 2.0 min) electrode with the charge transfer resistance decreased by 9.51 times, the inner active sites increased by 5.21 times and the ∙OH radicals generation ability enhanced by 4.07 times than the control EPD-0/PbO 2 anode. Consequently, the EPD-2.0/PbO 2 electrode achieved nearly 100% basic fuchsin (BF) and 86.78% COD removal efficiency after 3.0 h electrolysis. Therefore, this new PbO 2 electrode presented a promising potential for electrochemical degradation of BF and the new Ti 3 C 2 T x middle layer could also be used to fabricate other efficient and stable anodes, such as SnO 2 , MnO 2 , TiO 2 , etc.
研究领域:
环境科学
·
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
RSC Advances
·
2021
·Vol. 11
·期 46
·28949-28960
·
IF 3.361
Ze Lv,Zhen Chen,Qiang Yu,Wei Zhu,Hongjun You,Bangyao Chen,Zhaoyi Zheng,Yuanyuan Liu,Qi Hu
PbO2–Co3O4–MnO2 electrodes, used in the electrowinning industry and in the degradation of organic pollutants, have demonstrated an elevated performance through macroscopic electrochemical measurements. However, few reports have investigated localized electrochemical performance, which plays an indispensable role in determining the essential reasons for the improvement of the modified material. In this study, the causes of the increase in electrochemical reactivity are unveiled from a micro perspective through scanning electrochemical microscopy (SECM), X-ray diffraction (XRD), Raman microscopy (Raman), and X-ray photoelectronic energy spectroscopy (XPS). The results show that the increase of electrochemical reactivity of the modified electrodes results from two factors: transformation of the microstructure and change in the intrinsic physicochemical properties. Constant-height scanning maps indicate that the electrochemical reactivity of the modified electrodes is higher than that of the PbO2 electrode on the whole and high-reactivity areas are orderly distributed, coinciding with the observations from SEM and XRD. Thus, one of the reasons for the improvement of the modified electrode performance is the refinement of the microscopic morphology. The other reason is the surge of the oxygen vacancy concentration on the surface of the coating, which is supported by XRD, Raman and XPS. This finding is detected by the probe approach curve (PAC), which can quantitatively characterize the electrochemical reactivity of a substrate. Heterogeneous charge transfer rate constants of the modified electrode are 4–5 times higher than that of the traditional PbO2 electrode. This research offers some insight into the electrochemical reactivity of modified PbO2 electrodes from a micro perspective.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2022
·
IF 14.224
Xuanbing Wang,Junli Wang,Bohao Yu,Wenhao Jiang,Jinlong Wei,Buming Chen,Ruidong Xu,Linjing Yang
The oxygen evolution reaction kinetics in industrial zinc electrowinning is sluggish, resulting in low electrocatalytic activity and substantial energy expenditure (about one-third of energy was wasted due to the strong polarization effect). Herein, the paper described a core-shell structured MnCo 2 O 4.5 @C modified PbO 2 electrode through the pyrolysis and co-electrodeposition as a promising candidate for zinc electrowinning. As a result, the obtained Pb-0.2%Ag/ α -PbO 2 / β -PbO 2 -MnCo 2 O 4.5 @C composite electrode showed a sandwich-like structure, where Pb-0.2%Ag as a core, α -PbO 2 as a mid-layer, and β -PbO 2 -MnCo 2 O 4.5 @C served as an electrocatalytic layer. It also possessed improved OER catalytic activity , only required 680 mV to achieve a current density of 50 mA cm −2 and a Tafel slope of 216.04 mV dec −1 in an acidic solution containing 50 g L −1 Zn 2+ and 150 g L −1 H 2 SO 4 . The current efficiency increased by 0.7% and the cell voltage reduced by 360 mV as compared to a conventional Pb-0.76%Ag alloy electrode, leading to a remarkable energy-consumption reduction of 283.5 kW h for producing per ton metallic zinc. Furthermore, Pb-0.2%Ag/ α -PbO 2 / β -PbO 2 -MnCo 2 O 4.5 @C exhibited a prolonged service life, which worked about 44 h under an ultra-high current density of 2 A cm −2 . Hence, this paper provides the strategy to design and construct non-precious, high-performance catalyst for electrolysis and other applications.
研究领域:
材料科学
·
电化学
·
能源工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2015
·
IF 2.729
Yijing Xia,Qizhou Dai,Jianmeng Chen
The novel nickel modified PbO 2 electrodes were successfully prepared via electrodeposition in nitrate solution. The influence of nickel content on the physico-chemical properties and electrocatalytic performance of PbO 2 electrodes was investigated. The electrodes were characterized by SEM, EDX and XRD techniques. A limited amount of doping nickel could produce a more compact PbO 2 film and diminish the size of the crystal grains. The steady-state polarization curves and the cyclic voltammetry analysis showed that the 1% Ni–PbO 2 electrode had the highest oxygen evolution potential and the optimal electrochemical oxidation ability. The cyclic voltammograms with various scan rates showed that the oxidation of aspirin on these PbO 2 electrodes was a typical diffusion-controlled electrochemical process. Stability tests of different PbO 2 electrodes showed that 1% Ni–PbO 2 electrode had the highest electrochemical stability. In addition, nickel modified PbO 2 electrodes were used to degradation aspirin in aqueous solution, which gave the direct evidence of the electrocatalytic capabilities of these electrodes. The results showed that 1% Ni–PbO 2 electrode obtained the highest kinetic rate constant, chemical oxygen demand (COD) and total organic carbon (TOC) removals, which were 1.41, 1.22, 1.20 times than those of undoped PbO 2 electrode, respectively. Moreover, the energy required for the treatment of 1 m 3 aspirin solution significantly decreased and the hydroxyl radical utilization rate was enhanced after appropriate nickel doping. As a result, the 1% Ni–PbO 2 electrode is a promising anode for the treatment of organic pollutants.
研究领域:
环境科学
·
电化学
·
污染控制
✓ 已验证
DOI
高影响因子
Scientific Reports
·
2024
·Vol. 14
·期 1
·1-10
·
IF 3.8
Zhu Dancheng,Wu Yifan,Zheng Kai,Xu Hao,Chen Chao,Qiao Jun,Shen Chao
In this study, we deposited Ti 3 C 2 T x -modified, rare-earth-doped PbO 2 on the surface of a carbon fabric via electrodeposition. The surface morphology and electronic structure of the electrode were characterized with SEM, XRD and XPS. The layered Ti 3 C 2 T x did not change the structure of β-PbO 2 , and at the same time, it improved the crystallinity of the material and reduced the grains of PbO 2 . Electrochemical experiments showed that the addition of Ti 3 C 2 T x increased the electrochemical activity of the electrode and produced more H 2 O 2 , which contributed to the degradation of pollutants. The efficiency of sulfamethoxazole (SMX) degradation reached 95% after 120 min at pH 3 with a current density of 50 mA/cm 2 . Moreover, the electrode has good cycling performance, and the degradation efficiency was still 80% after 120 min after 10 cycles of recycling. Based on the intermediates identified by HPLC‒MS, a mechanism for SMX degradation was proposed. Our results will provide a new idea for the development of efficient electrocatalytic degradation of antibiotics.
研究领域:
环境科学
·
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMOSPHERE
·
2018
·
IF 4.427
Yijing Xia,Qizhou Dai
In this work, the electrochemical degradation of antibiotic levofloxacin (LFX) has been studied using a novel rare earth La, Y co-doped PbO 2 electrode. The effect of applied current density, pH value and initial LFX concentration on the degradation performance were systematically evaluated. The results demonstrated that electrochemical oxidation of LFX over the La-Y-PbO 2 electrode was highly effective and the reaction followed an apparent first-order kinetic model. Considering the degradation efficiency and energy efficiency, the relative optimal conditions are identified as current density 30 mA cm −2 , pH 3 and initial LFX concentration 800 mg L −1 . According to the identified products, a reaction mechanism has been proposed and the products were further oxidized to CO 2 , H 2 O, NH 4 + , NO 3 − and F − . A total of four aromatic intermediate products of LFX degradation were identified and the different structural changes to the LFX molecule included pepiperazinyl hydroxylation, decarboxylation and defluorination .
研究领域:
环境科学
·
电化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2016
·
IF 3.299
Qizhou Dai,Jiazhong Zhou,Mili Weng,Xubiao Luo,Daolun Feng,Jianmeng Chen
This study presents an electrochemical method for the degradation of metronidazole (MNZ) in aqueous solution with novel PbO 2 electrode, which was prepared via electrodeposition in nitrate solution. The influencing factors on electrochemical decomposition of pollutants were evaluated and the removal of MNZ and chemical oxygen demand (COD) reached 78.09% and 21.77% after 120 min treatment under the optimal conditions with the concentration of supporting electrolyte, the initial concentration of MNZ, the pH and the current density were 0.10 mol/L, 100 mg/L, 6.4 and 10 mA/cm 2 , respectively. Then, the Co doped PbO 2 electrodes were prepared and used to degrade MNZ under the optimal conditions. Relatively good performance was achieved when the molar ratio of Pb and Co was 100:1. Compared to pure PbO 2 electrode, the steady-state polarization curves and cyclic voltammetry analysis showed that 1.0% Co-PbO 2 electrode had a higher oxygen evolution potential and greater current of reduction and oxidation peaks, which increased the electrochemical activity and decreased the energy consumption. Finally, based on the intermediate products identified by IC and GC/MS, the main degradation pathway of MNZ was proposed including ring open, denitrification and radical reactions.
研究领域:
环境科学
·
电化学工程
✓ 已验证
DOI
高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2021
·Vol. 168
·期 10
·106510
·
IF 4.316
Yijing Xia,Yan Yan,Lingbing Hu,Qizhou Dai,Xiangjuan Ma,Juqing Lou,Yi Xia
This study focused on the enhanced mechanism of electrochemical degradation of antibiotic norfloxacin (NOR) using a self-made Ti/SnO2-Sb2O3/α,β-Co-PbO2 electrode. The electrode characterization, reaction mechanism, degradation performance, and toxicity assessment were studied. In contrast to the conventional Ti/SnO2-Sb2O3/α,β-PbO2 electrode, our prepared Co-doped PbO2 electrode showed the characteristics of more compact surface, smaller crystal size, higher oxygen evolution potential (OEP) and an increased yield of ·OH concentration. The application of Co-doped PbO2 electrode for the electrochemical oxidation of NOR was systematically analyzed. The optimal operating parameters were found to be Na2SO4 concentration of 0.1 mol L−1, initial NOR concentration of 50 mg L−1, initial pH of 5 and current density of 20 mA cm−2. Under these conditions, NOR, chemical oxygen demand (COD) and total organic carbon (TOC) removals reached 85.29%, 43.65% and 41.89% after 60 min of electrolysis, respectively. Through the intermediates detected during the electrochemical treatment process, a reaction pathway involving decarboxylation, defluorination and piperazine ring-opening was proposed. Finally, the toxicity assessment of the treated NOR solution towards Vibrio fischeri rapidly fell to non-toxicity and even reached to negative values after 50 min of electrolysis, indicating that electrochemical oxidation of NOR is an effective approach to reduce its toxicity to environmental ecosystem.
研究领域:
环境科学
·
电化学工程
·
毒理学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2022
·
IF 4.598
Jieqi Feng,Hao Lan,Qibin Tao,Wenqing Chen,Qizhou Dai
In this study, a novel NCNS-Ce-PbO 2 electrode was prepared by electrodeposition method using the rare earth metal Ce and synthesized nitrogen-doped carbon nanosheets (NCNSs). Various characterization and electrochemical performance tests showed that the NCNS-Ce-PbO 2 electrode possessed a denser surface and smaller grains than other NCNS-PbO 2 and Ce-PbO 2 electrodes, with more active surface sites and thus could generate more hydroxyl radicals. N , N -diethyl-m-toluamide (DEET) was selected as the model contaminant to evaluate the electrochemical performance of the novel NCNS-Ce-PbO 2 electrode. The effects of initial pollutant concentration, current density, electrolyte concentration, and initial pH on the removal rates of DEET and chemical oxygen demand (COD) were investigated. Under optimal conditions, after degradation of 150 min, the removal rate of DEET and COD reached 100% and 80.52%, respectively. GC–MS was used to identify intermediate products in the degradation process. The degradation mechanism and possible degradation pathways of DEET with NCNS-Ce-PbO 2 electrode were discussed. The good stability of the NCNS-Ce-PbO 2 anode was confirmed by accelerated lifetime experiments.
研究领域:
环境科学
·
电化学工程
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）