JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2020
·Vol. 167
·期 14
·142505
·
IF 3.721
Wei Han,Wenjuan Wang,Mei Li,Yangyang Meng,Wenjing Ji,Yang Sun
To recover Gd from LiCl-KCl eutectic, the coreduction mechanism of Gd(III) with Pb(II) was investigated using electrochemical methods. The formation potentials related to the formation of three Gd-Pb intermetallics were detected by cyclic voltammetry, square wave voltammetry and chronopotentiometry, and the formation mechanism of Gd-Pb compounds could be described as xPb(II) + 2xe− = xPb. Meanwhile, the electroreduction of Gd on liquid Pb electrode was explored. The diffusion coefficient of Gd metal in liquid metallic Pb was determined by anodic chronopotentiometry. The kinetic parameters of Gd(III)/Gd(in Pb) couple in the temperature range from 723 K to 873 K were determined employing linear polarization (LP) method. Based on the relationship of exchange current density and temperature, the reaction activation energy was estimated to be 23.17 kJ mol−1. In addition, the recovery of Gd from molten salts was performed assisted by liquid Pb electrode by constant potential electrolysis (CPE) and constant current electrolysis (CCE). The products characterized using XRD, SEM with EDS are comprised of GdPb3 and Pb phases. The concentration change of Gd during CCE process was monitored by ICP-AES, and the recovery rate was estimated. The results showed that Gd concentration decreased and recovery rate increased with the duration.
研究领域:
材料科学
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电化学工程
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DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Lina Zhang,Xin Li,Lihui Chen,Chunyang Zhai,Hengcong Tao
The electrochemical CO 2 reduction (ECR) of high-value multicarbon products is an urgent challenge for catalysis and energy resources. Herein, we reported a simple polymer thermal treatment strategy for preparing honeycomb-like CuO@C catalysts for ECR with remarkable C 2 H 4 activity and selectivity. The honeycomb-like structure favored the enrichment of more CO 2 molecules to improve the CO 2 -to-C 2 H 4 conversion. Further experimental results indicate that the CuO loaded on amorphous carbon with a calcination temperature of 600 °C (CuO@C-600) has a Faradaic efficiency (FE) as high as 60.2% towards C 2 H 4 formation, significantly outperforming pure CuO-600 (18.3%), CuO@C-500 (45.1%) and CuO@C-700 (41.4%), respectively. The interaction between the CuO nanoparticles and amorphous carbon improves the electron transfer and accelerates the ECR process. Furthermore, in situ Raman spectra demonstrated that CuO@C-600 can adsorb more adsorbed *CO intermediates, which enriches the C C coupling kinetics and promotes C 2 H 4 production. This finding may offer a paradigm to design high-efficiency electrocatalysts, which can be beneficial to achieve the “double carbon goal.”
研究领域:
催化
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能源材料
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环境科学
✓ 已验证
DOI
高影响因子
Nature Communications
·
2025
·Vol. 16
·期 1
·1-13
·
IF 15.7
Cheng Qiyang,Liu Sisi,He Yanzheng,Wang Mengfan,Ji Haoqing,Huan Yunfei,Qian Tao,Yan Chenglin,Lu Jianmei
The direct synthesis of ammonia from nitrate (NO 3 – ) reduction in acid is a promising approach for industrialization. However, the difficulty arises from the intense competition with the inevitable hydrogen evolution reaction, which is favoured due to the overwhelming protons (H + ). Here, we systematically explore and rationally optimize the microenvironment using multivariate covalent organic frameworks (COFs) as catalyst adlayers to promote the nitrate-to-ammonia conversion in acid. With the application of tailored positive electrostatic potential generated over the multivariate COFs, both the mass transfer of NO 3 – and H + are regulated via appropriate electrostatic interactions, thus realizing the priority of NO 3 RR with respect to HER or NO 3 – -to-NO 2 – . As a result, an NH 3 yield rate of 11.01 mmol h –1 mg –1 and a corresponding Faradaic efficiency of 91.0% are attained, and solid NH 4 Cl with a high purity of 96.2% is directly collected in acid; therefore, this method provides a practical approach for economically valorising wastewater into valuable ammonia.
研究领域:
材料科学
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环境科学
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电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Yi-Hong Yu,Xin Cui,Yi-Meng Hong,Gao-Wu Qin,Song Li
Incorporating electrochemical CO 2 reduction (ECR) that produces CO-rich syngas into the workflow of steelmaking presents a promising strategy to neutralize the steelmaking industry. Herein, we develop a highly efficient and stable Ag nanowires with surface CeO 2 armors (CeO 2 /AgNWs) as ECR electrocatalyst for syngas production. The engineered CeO 2 -Ag interface facilitates CO 2 -to-CO conversion by lowering the energy barrier for *COOH intermediate formation through synergistic electronic effects. At an industrially relevant current density of −251.3 mA cm −2 , the CeO 2 /AgNWs generate CO-rich syngas by co-electrolysis of CO 2 and H 2 O, with a high Faradaic efficiency (FE) of 92.1 % for CO. Techno-economic analysis (TEA) reveals that integrating the CeO 2 /AgNWs-driven ECR into existing steelmaking workflows can potentially reduce CO 2 emissions by 83 % and elevate the renewable energy utilization to ∼91.4 %, unlocking new possibilities for achieving carbon neutrality in the steel industry.
研究领域:
材料科学
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能源工程
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
ChemistrySelect
·
2024
·Vol. 9
·期 22
·e202401690
·
IF 1.9
Menghan Xue,Fazhan Li,Zhen Li,Yuxia Sun,Yiping Guo,Yuehui Li
Graphical Increase of graphitic-N doping and graphitization degree of outside shells encapsulating Ni nanoparticles was developed to efficiently promote cathodic reduction of CO 2 to CO. Despite of high conductivity and reducing ability, transition metal nanoparticles tend to aggregate and unavoidably impact the selectivity during the proton-coupled reduction process of CO 2 RR. New strategy to regulate and utilize the electronic property of transition-metal particles allows for effective tuning of eCO 2 RR activity. Through simple creation of N-doped carbon shells surrounding Ni nanoparticles and controlling the amount and arrangement of the N atoms, successful and long-lasting electrochemical reduction of CO 2 was accomplished. The inherent HER activity was almost completely suppressed. It exhibited FE CO above 90 % in a 500 mV potential window, with the optimal up to 96.5 % at −0.78 V vs RHE. In flow cell electrolysis, a current density of 289.4 mA/cm 2 was achieved with Faradic efficiency of 96.4 % towards CO. The results of control experiments using different catalysts imply that electron transfer between Ni core and shells was significantly influenced by the property of N atoms. High content of graphitic nitrogen is crucial for the catalytic performance.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2019
·Vol. 166
·期 2
·B35
·
IF 3.12
Juanjuan Gao,Weiqing Zhu,Haiou Song,Shupeng Zhang
p-Phenylenediamine (PPD) and hydroquinone (HQ) are hair dye precursors for permanent dyeing and are used globally. We report a novel and economic approach for the selective and simultaneous detection of the cathodic peaks of PPD and HQ by using a bare glassy carbon electrode, compared with modified electrodes that are obtained by tedious or expensive functionalized and that failed to achieve a peak-to-peak separation of PPD and HQ. Linear relationships between the simultaneous cathodic peak current of PPD and HQ concentrations were obtained for 0.5–400 μM and 5–4,000 μM with detection limits (S/N = 3) of 0.163 and 0.353 μM, respectively. The glassy carbon electrode sensor was applied to determine PPD and HQ in Nanjing river water with a recovery for these two analogues of 98.7–103.9% and 98.0–102.4%, respectively.
研究领域:
分析化学
·
环境科学
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
·
IF 19.503
Ke Ye,Tianfu Liu,Yanpeng Song,Qi Wang,Guoxiong Wang
Electrochemical CO 2 reduction reaction (CO 2 RR) offers an appealing route to simultaneously store intermittent renewable energy as value-added chemicals and close carbon cycle. Silver (Ag) catalyst is a promising candidate for the electrochemical conversion of CO 2 to CO, but the electrocatalytic properties are still insufficient for practical applications. Herein, we put forward a strategy to in situ reconstruct a heterogeneous Ag 2 S/Ag interface structure, in which their strong interactions facilitate CO 2 RR performance. The in situ reconstructive Ag 2 S/Ag catalyst achieves a large current density of 421.7 ± 14.4 mA cm –2 at –0.70 V vs . reversible hydrogen electrode (RHE) and maintains steadily at a current density of 244.5 ± 31.8 mA cm –2 and CO Faradaic efficiency of 99.1 ± 0.8 % at –0.49 V vs . RHE for 50 h, superior to state-of-the-art CO-selective Ag-based catalysts. Density functional theory calculations reveal that the in situ reconstructive Ag 2 S/Ag interface active sites stabilize the *COOH intermediate during CO 2 RR process.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Energy Chemistry
·
2020
·
IF 7.216
Hui Ning,Dianliang Guo,Xiaoshan Wang,Zhonghao Tan,Wenhang Wang,Zhongxue Yang,Linqing Li,Qingshan Zhao,Jian Hao,Mingbo Wu
Developing of economic and efficient catalysts is critical for the application of electroreduction of carbon dioxide to highly valuable chemicals. Herein, we present a facile method to synthesize N-doped hieratically porous carbon through pyrolysis of petroleum pitch followed by ammonia etching. We found mesopores are favored formation by removing of asphaltene from petroleum pitch during the carbonation process. Simultaneously, ammonia etching can not only increase the pyridinic-N content, but also upgrade the ratio of meso- to micro- pores of carbon materials. Using the N-doped hieratically porous carbon as catalyst for carbon dioxide electroreduction, the Faradaic efficiency of carbon monoxide reaches 83% at −0.9 V vs. the reversible hydrogen electrode (RHE) in 0.1 M KHCO 3 . This superior performance is attributed to the synergistic effects of highly pyridinic-N content in conjunction with the hieratically porous architecture, rendering abundant exposed and accessible active sites for electroreduction of CO 2 . Our work provides a new strategy for the large-scale preparation of high-performance, low-cost catalysts for CO 2 electroreduction.
研究领域:
材料科学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
Greenhouse Gases-Science and Technology
·
2021
·Vol. 11
·期 6
·1191-1197
·
IF 2.013
Subrato Acharjya,Jiacheng Chen,Minghui Zhu,Chong Peng
Immobilized tin phthalocyanine dichloride (SnPcCl 2 ) was prepared by refluxing SnPcCl 2 and hydroxyl-functionalized carbon nanotubes in DMF with the addition of triethylamine, which exhibited minimal aggregation and approximately 2–3 folds improvement in activity towards CO 2 electroreduction compared to the physically mixed SnPcCl 2 /CNT hybrid. Cyclic voltammetry analysis and in situ UV-vis spectra revealed that metallic tin is the active site for CO 2 electroreduction, and the redox behavior of Sn 0 is affected by the adjacent demetallized macrocycles. © 2021 Society of Chemical Industry and John Wiley & Sons, Ltd.
研究领域:
材料科学
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电化学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2015
·
IF 1.964
Yanyan Xu,Mingming Gao,Guohui Zhang,Xinhua Wang,Jiajia Li,Shuguang Wang,Yuanhua Sang
An electrochemically reduced graphene oxide sample, ERGO -0.8V , was prepared by electrochemical reduction of graphene oxide (GO) at –0.8 V, which shows unique electrocatalytic activity toward tetracycline (TTC) detection compared to the ERGO -1.2V (GO applied to a negative potential of –1.2 V), GO, chemically reduced GO (CRGO)-modified glassy carbon electrode (GC) and bare GC electrodes. The redox peaks of TTC on an ERGO -0.8V -modified glass carbon electrode (GC/ERGO -0.8V ) were within 0–0.5 V in a pH 3.0 buffer solution with the oxidation peak current correlating well with TTC concentration over a wide range from 0.1 to 160 mg/L. Physical characterizations with Fourier transform infrared (FT-IR), Raman, and X-ray photoelectron spectroscopies (XPS) demonstrated that the oxygen-containing functional groups on GO diminished after the electrochemical reduction at –0.8 V, yet still existed in large amounts, and the defect density changed as new sp 2 domains were formed. These changes demonstrated that this adjustment in the number of oxygen-containing groups might be the main factor affecting the electrocatalytic behavior of ERGO. Additionally, the defect density and sp 2 domains also exert a profound influence on this behavior. A possible mechanism for the TTC redox reaction at the GC/ERGO -0.8V electrode is also presented. This work suggests that the electrochemical reduction is an effective method to establish new catalytic activities of GO by setting appropriate parameters.
研究领域:
分析化学
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环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
Catalysts
·
2021
·Vol. 11
·期 11
·1349
·
IF 4.146
Liaochuan Jiang,Xingyuan Gao,Shaoling Chen,Jangam Ashok,Sibudjing Kawi
At present, TiO2is one of the most widely used photocatalytic materials. However, the narrow response range to light limits the photocatalytic performance. Herein, we reported a successful construction of self-doped R-WO3/R-TiO2/CC nanocomposites on flexible carbon cloth (CC) via electrochemical reduction to increase the oxygen vacancies (Ovs), resulting in an enhanced separation efficiency of photo-induced charge carriers. The photocurrent of R-WO3/R-TiO2/CC at −1.6 V (vs. SCE) was 2.6 times higher than that of WO3/TiO2/CC, which suggested that Ovscould improve the response to sunlight. Moreover, the photocatalytic activity of R-WO3/TiO2/CC was explored using methylene blue (MB). The degradation rate of MB could reach 68%, which was 1.3 times and 3.8 times higher than that of WO3/TiO2/CC and TiO2/CC, respectively. Furthermore, the solution resistance and charge transfer resistance of R-WO3/R-TiO2/CC were obviously decreased. Therefore, the electrochemical reduction of nanomaterials enabled a promoted separation of photogenerated electron–hole pairs, leading to high photocatalytic activity.Keywords:photocatalysis;electrochemical reduction;photocatalytic degradation;TiO2;WO3
研究领域:
材料科学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
ChemSusChem
·
2022
·Vol. 15
·期 8
·e202200090
·
IF 9.14
Wenwen Bao,Senhe Huang,Diana Tranca,Boxu Feng,Feng Qiu,Fermín Rodríguez-Hernández,Changchun Ke,Sheng Han,Xiaodong Zhuang
Graphical Beauty in balanced asymmetry : An asymmetric Co II porphyrin ( as -PorCo) is constructed with a substituent of 2,6-dimethylbenzene to enhance the charge transfer capability from carbon nanotubes to as -PorCo, resulting in large partial current density of 8 mA cm −2 and high turnover frequency of 5656 h −1 at −0.7 V vs. reversible hydrogen electrode in aqueous solution. The present study provides the new insight into molecular design of catalysts for efficient electrochemical CO 2 reduction. The electrochemical reduction of carbon dioxide (CO 2 ) based on molecular catalysts has attracted more attention, owing to their well-defined active sites and rational structural design. Metal porphyrins (PorMs) have the extended π-conjugated backbone with different transition metals, endowing them with unique CO 2 reduction properties. However, few works focus on the investigation of symmetric architecture of PorMs as well as their aggregation behavior to CO 2 reduction. In this work, a series of Co II porphyrins (PorCos) with symmetric and asymmetric substituents were used as model of molecular catalysts for CO 2 reduction. Owing to the electron donating effect of 2,6-dimethylbenzene (DMB), bandgaps of the complexes became narrower with the increasing number of DMB. As electrocatalysts, all PorCos exhibited promising electrocatalytic CO 2 reduction performance. Among the three molecules, asymmetric Co II porphyrin ( as -PorCo) showed the lowest onset potential of −288 mV and faradaic efficiencies exceeding 93 % at −0.6 V vs. reversible hydrogen electrode, which is highly competitive among the reported state-of-art porphyrin-based electrocatalysts. The CO 2 reduction performance depended on π-π stacking between PorCo with carbon nanotubes (CNTs) and adjacent PorCos, which could be readily controlled by atomically positioned DMB in PorCo. Density functional theory calculations also suggested that the charge density between PorCo and CNT was highest due to the weak steric hindrance in as -PorCo, providing the new insight into molecular design of catalysts for efficient electrochemical CO 2 reduction.
研究领域:
催化化学
·
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）