ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2021
·
IF 9.028
Bo Zhang,Jing Bai,Yan Zhang,Changhui Zhou,Pengbo Wang,Lina Zha,Jinhua Li,Abdolreza Simchi,Baoxue Zhou
H2S and CO2 are the main impurities in raw natural gas, which needs to be purified before use. However, the comprehensive utilization of H2S and CO2 has been ignored. Herein, we proposed a fully resource-based method to convert toxic gas H2S and greenhouse gas CO2 synchronously into CO and elemental S by using a novel electrochemical reactor. The special designs include that, in the anodic chamber, H2S was oxidized rapidly to S based on the I–/I3– cyclic redox system to avoid anode passivation. On the other hand, in the cathodic chamber, CO2 was rapidly and selectively reduced to CO based on a porous carbon gas diffusion electrode (GDE) modified with polytetrafluoroethylene and cobalt phthalocyanine (CoPc). A high Faraday efficiency (>95%) toward CO was achieved due to the enhanced mass transfer of CO2 on the GDE and the presence of the selective CoPc catalyst. The maximum energy efficiency of the system was more than 72.41% with a current density of over 50 mA/cm2, which was 12.5 times higher than what was previously reported on the H2S treatment system. The yields of S and CO were 24.94 mg·cm–2·h–1 and 19.93 mL·cm–2·h–1, respectively. A model analysis determined that the operation cost of the synchronous utilization of H2S and CO2 method was slightly lower than that of the single utilization of H2S in the existing natural gas purification technology. Overall, this paper provides efficient and simultaneous conversion of H2S and CO2 into S and CO.
研究领域:
环境科学
·
能源化学
✓ 已验证
DOI
高影响因子
Energy Storage Materials
·
2018
·
IF 0
Qian Liang,Fuming Chen,Shaofeng Wang,Qiang Ru,Qinyu He,Xianhua Hou,Ching-yuan Su,Yumeng Shi
Renewable energy-related technologies have become more important due to the increasing energy consumption. Herein, we put forward a novel organic flow desalination battery (ORFDB) using redox-active organic molecule electrolyte materials dissolved in the aqueous sodium chloride feed. Riboflavin-5’-phosphate sodium salt dihydrate (FMN-Na) is used as the anolyte, and the catholyte is 4-hydroxy-2,2,6,6-tetramethylpiperidin-1-oxyl (TEMPO). Sodium and chloride ions in salt feed were moved respectively to anolyte and catholyte by electrochemical reaction of electrolytes during the charge process, and return to the feed during the discharge process. This ORFDB system possesses the stable stability up to fifty cycles and the excellent rate performance. This ORFDB exhibits the cost-effective renewable energy storage and the possibility of salt removal based on the electrochemistry of organic molecules.
研究领域:
能源科学
·
电化学
·
材料科学
✓ 已验证
产品关联
DOI
ACS Earth and Space Chemistry
·
2024
·
IF 2.9
Junqi Ren,Wenshuo Mao,Zhongchen Wu,Xiaohui Fu,Qiyuan Hou,Mingyu Chen,Ziwei Fu
The Martian atmosphere and surface materials can be impacted by electrochemical reactions that occur during dust activity on Mars. Prior research has shown that in the dry Martian surface environment, electrostatic discharge (ESD) can generate oxychlorine along with converting CO2 to carbonate dust. To comprehend the carbon and chlorine cycles on Mars, research on carbonates and oxychlorine is crucial, as is investigating the effects of coexisting minerals. In support of this work, precise methods for measuring ESD reactions are needed. Herein, ESD reactions on chloride (NaCl) and potential coexisting minerals SiO2 or TiO2 were investigated under simulated Martian atmosphere conditions, and Raman spectroscopy was used to measure trace products. Based on Raman measurements, the influences of coexisting minerals on the production of carbonates and oxychlorine during ESD reactions were investigated. Our findings suggest that Raman spectroscopy has sensitive quantitative detection capabilities in aqueous solutions, offering a useful technique for the quantitative detection of laboratory products. Carbonate continuously accumulated with increasing discharge time, with 14–22 times greater yield (1.43–4.77‰ and 5% error) than perchlorate (0.10–0.24‰ and 20% error) and 5–16 times greater yield than chlorate (0.28–0.44‰ and 20% error). The yields of the above products were found to depend on the type, content, and particle size of coexisting minerals. Our findings are crucial for understanding the current geological history, atmospheric evolution, and substance cycling on Mars, as well as for retracing the development of Martian atmospheric and hydrological environments.
研究领域:
行星科学
·
地质学
·
化学
✓ 已验证
DOI
高影响因子
Journal of Materials Research and Technology-JMR&T
·
2022
·
IF 6.267
Jun Chen,Yan Zhao,Mingchen Sun,Zhiwei Liu,Hansong Liu,Shu Xiong,Shuang Li,Jiupeng Song,Kai Wang
In this study, a simple and rapid grafting method, without damage to carbon fiber (CF), is proposed to graft MXene nanosheets onto the surface of CF via covalent bonds through electrochemical aryldiazonium salt reaction and using p-phenylenediamine molecule as a bridge so as to enhance the interfacial properties of CF/epoxy (EP) composites. The surface morphology , chemical activity and wettability of the modified CF were characterized by scanning electron microscope, atomic force microscopy , X-ray photoelectron spectroscopy and dynamic contact angle test. The effect of such surface modification method on the mechanical properties was also evaluated. Compared with untreated CF, the interfacial shear strength of MXene functionalized CF reached 123.86 MPa, increasing by 33.5% while the tensile strength is not reduced. The interfacial enhancement mechanism might be the strong physical and chemical interactions between MXene and EP resin matrix produced by the rough structure and high surface activity of MXene. This work may provide a new idea with a facile and rapid approach to modify the surface of CF and improve the interfacial properties of composites without degrading the mechanical property of pristine CF.
研究领域:
材料科学
·
复合材料
✓ 已验证
产品关联
DOI
高影响因子
Journal of Energy Chemistry
·
2025
·
IF 14.9
Rui Xue,Shu Yuan,Rongyi Wang,Tianzi Bi,Guiru Zhang,Huiyuan Li,Jiewei Yin,Liuxuan Luo,Shuiyun Shen,Xiaohui Yan,Junliang Zhang
With the development of renewable energy, electrochemical carbon dioxide reduction reaction (CO 2 RR) has become a potential solution for achieving carbon neutrality. However, until now, due to issues with salt precipitate and regeneration of the electrolyte, this technology faces challenges such as difficulty in maintaining long-term stable operation and excessive costs. The pure water CO 2 electrolyzers are believed to be the ultimate solution to eliminate the salt depreciation and electrolyte issues. This study develops an in-situ method tailored for CO 2 reduction in pure water. By employing distribution of relaxation times (DRT) analysis and in-situ electrochemical active surface area (ECSA) measurements, we carried out a comprehensive investigation into the mass transport and electrochemical active surface area of gas diffusion electrodes (GDE) under pure water conditions. The maximum 89% CO selectivity and high selectivity (>80%) in the range of 0–300 mA/cm 2 were achieved using commercial Ag nanoparticles by rational design of catalyst layer. We found that ionomers influence the CO 2 electrolyzers performance via affecting local pH, GDE-membrane interface, and CO 2 transport, while catalyst loading mainly influences the active area and CO 2 transport. This work provides benchmark and insights for future pure water CO 2 electrolyzers development.
研究领域:
能源科学
·
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2023
·
IF 4.5
Biwu Cai,Jianbang Ge,Fei Zhu,Yang Gao,Shuqiang Jiao
Natural convection could arise under density gradients of solutions caused by the electrochemical reaction occurring on the electrode surface. This density-driven convection decays rapidly with the decreasing redox concentration, and becomes negligible in dilute solutions (1–2 mM). However, steady-state voltammetry is still observed in these dilute solutions due to the presence of a convection–diffusion layer. Here we studied natural convection effects in low-concentration (5–30 mM) redox solutions and clarified the convection modes in these transient-concentration solutions using cyclic voltammetry and chronoamperometry. The combined theoretical–experimental work demonstrated the coexistence of convection–diffusion layer and density-driven convection. With the use of a 150-μm-radius Pt microelectrode, the convection–diffusion layer convection dominated natural convection in dilute solution (1–5 mM), reinforced mass transport with density-driven convection in low redox concentrations (5–11 mM), and suppressed the density-driven convection at high redox concentrations (>15 mM). The zone diagrams delineating the transition from diffusion to convection were then established to reveal the effects of electrode radius, thickness of the convection–diffusion layer, time scale, and redox concentration on natural convection. Consequently, the use of microelectrodes (∼25 μm radius) could greatly inhibit natural convection effects in 30 mM redox solution.
研究领域:
电化学
·
传质工程
·
物理化学
✓ 已验证
产品关联
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2022
·Vol. 32
·期 20
·2112113
·
IF 19.924
Zhonghui Gao,Yang Bai,Haoyu Fu,Jiayi Yang,Thimo Ferber,Junrun Feng,Wolfram Jaegermann,Yunhui Huang
Garnet-type Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 (LLZTaO) is considered a promising solid-state electrolyte (SSE) for all-solid-state batteries (SSBs), but LLZTaO/Li interfacial issues limit their power density. The key question of whether LLZTaO does or does not form an interphase layer before and at the initial stage of electrochemical cycling remains debatable. An XPS interface approach, electrochemical cycling, and an electrochemically coupled phase field model to study the dynamic changes of interfacial resistance during cycling are utilized, and it is found that the generation rate of the interphase via electrochemical reaction processes at the LLZTaO/Li interface depends on the applied current density. For a Li/LLZTaO/Li cell, the impedance and overpotential increase gradually at the initial stage of electrochemical cycling at a current density of 0.1 mA cm –2 due to the formation of a passivating reaction zone (interphase) at LLZTaO/Li interface, which can protect the LLZTaO from being continuously reacted. With increasing the current density to 0.5 mA cm –2 , the electrochemical reaction is suppressed and tied to uneven Li ion transport across the LLZTaO/Li interface on plating, leading to a short circuit of the cell. Understanding how interface dynamic transformations influence electrochemical degradation is helpful to stabilize these interfaces in SSBs.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
DOI
高影响因子
Materials Horizons
·
2025
·
IF 10.7
Mengjie Si,Yueman Tang,Chen Xu,Chen Yu Li,Kaishun Xia,Wei Xu,Ji Lin,Zhen Jiang,Jintao Yang,Si Yu Zheng
Developing hydrogels with high conductivity and toughness via a facile strategy is important yet challenging. Herein, we proposed a new strategy to develop conductive hydrogels by growing metal dendrites. Water-soluble Sn2+ ions were soaked into the gel and then converted to Sn dendrites via an electrochemical reaction; the excessive Sn2+ ions were finally removed by water dialysis, accompanied by dramatic shrinkage of the gel. Based on in situ transformation from metal ions to dendrites, the method integrated the advantages of ionic conductive fillers, such as LiCl (uniform dispersion), and electrical fillers, such as metal particles (high conductivity). Additionally, the morphology of metal dendrites combined advantages of 1D nanowires (large aspect ratio of the branches) and 2D nanosheets (large specific surface area of the skeleton). The strategy was found to be effective across diverse gel systems (non-ionic, anionic, cationic and zwitterionic). The dense, highly conductive and branched Sn dendrites not only formed a conductive pathway but also interacted with the polymer network to transfer stress and dissipate energy. The resultant gel exhibited a high conductivity of 12.5 S m−1, fracture energy of 1334.0 J m−2, and fatigue threshold of 720 J m−2. Additionally, the gel exhibited excellent sensitivity when used as a wearable strain sensor and bioelectrode. We believe this strategy offers new insights into the development of conductive hydrogels.
研究领域:
材料科学
·
生物医学工程
·
化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
TALANTA
·
2025
·
IF 6.1
Chen Zeng,Jianxiong Chen,Chengbiao Zhu,Zhenwei Wei
Capturing and analyzing low-abundance, short-lived, and unstable radical intermediates during electrochemical (EC) reactions is important for understanding EC reaction mechanisms. Herein, we developed a chemical labeling strategy for rapid screening and highly sensitive analysis of EC radical intermediates by mass spectrometry (MS). Taking 5,5-dimethyl-1-pyrroline N-oxide (DMPO) labeling reagent as an example, DMPO can react with radical intermediates to form stable labeling products with characteristic fragmentation daughter ions or neutral loss in tandem MS, so the labeled intermediates can be screened by precursor ions scan or neutral loss scan. Further combined with our recently established floating electrochemical electrospray mass spectrometry platform (FE-ESI-MS), we realized online confirmation and in-depth analysis of radical intermediates, and accelerated the study of EC reaction mechanisms. We established the strategy based on the labeling analysis of radical intermediates produced by EC oxidation of acetaminophen and a mixed EC reaction system containing 10 substrates, and further studied the radical-radical cross coupling mechanism of sodium p -toluenesulfinate and 2-methyl-2H-indazole. The labeled products not only improved the MS response by more than 10 times, but also exhibited typical fragmentation behavior, which contributed to the rapid screening of radical intermediates. This chemical labeling strategy will increase the capability of MS for finding important EC intermediates in untargeted analysis and further investigating low abundant and short-lived EC intermediates in the future.
研究领域:
分析化学
·
电化学
·
质谱学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 48
·期 3
·1233-1240
·
IF 3.3
Li Ding,Xin Kong,Yan Gong,Shanxin Yang,Yongde Yan,Yuan Deng,Yun Xue,Kai Zhu,Fuqiu Ma,Wei Liu
Bismuth (Bi) is a potential cathode material to drive the development of Gd extraction by molten salt electrolysis. However, study on the electrolytic reduction of Gd by Bi electrode in melts has not receive sufficient attention and understanding. Therefore, in this work, the electrochemical reactions, kinetic processes and thermodynamic properties in the electrolytic extraction of Gd were investigated by various electrochemical methods. The electrochemical results showed that only two Gd–Bi alloys were formed in the electrode reaction. Moreover, the exchange current density and activity coefficient during electrolysis were determined by galvanostatic pulse (GP) and Coulomb titration, respectively. The temperature dependence of both exchange current density and activity coefficient was further revealed. Finally, Gd was successfully extracted in the form of alloys through potentiostatic electrolysis.
研究领域:
冶金学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
Chemical Science
·
2021
·Vol. 12
·期 27
·9494-9499
·
IF 9.825
Jilin Liu,Kai Yu,Hong Zhang,Jing He,Jie Jiang,Hai Luo
Towards the goal of on-line monitoring of transient neutral intermediates during electrochemical reactions, an electrochemistry-neutral reionization-mass spectrometry (EC-NR-MS) technique was developed in this work. The EC-NR setup consisted of a customized EC flow cell, a sonic spray ionization source, a heating tube, an ion deflector and an electrospray ionization source, which were respectively used for the precise control of the electrochemical reaction, solution nebulization, droplet desolvation, ion deflection and neutral intermediate ionization. Based on the EC-NR-MS approach, some long-sought neutral radicals including TPrA˙, DBAE˙ and TEOA˙, which belong to important reductive intermediates in electrochemiluminescence (ECL) reactions, were successfully identified which helps to clarify the previously unproven ECL reaction mechanism. These findings were also supported by spin-trapping experiments and the tandem MS technique. Accordingly, the EC-NR-MS method provides a direct solution for studying complicated electrochemical reactions, especially for detecting short-lived neutral radicals as well as ionic intermediates.
研究领域:
分析化学
·
电化学
·
质谱分析
✓ 已验证
DOI
PubMed
高影响因子
GREEN CHEMISTRY
·
2024
·
IF 9.3
Yuefeng Qiu,Peng Jiang,Wenkai Ye,Jiahao Hu,Bin Zhang,Tuo Ji,Liwen Mu,Xin Feng,Xiaohua Lu,Jiahua Zhu
An electrochemical–thermal tandem reaction system was designed in this work and enabled the highly efficient synthesis of propylene oxide (PO) at 1 atm without the use of H2O2. The electrochemical part produced OOH− through a 2e− oxygen reduction reaction, which migrated and distributed in the full space of a chamber filled with a mixture of solid electrolyte particles and modified TS-1 (m-TS-1) catalysts. Mediated by the relay of OOH− and protic solvent methanol, full space tandem reactions were achieved with a high PO selectivity of 95.2% and a productivity of 319.75 mmol gecat−1 h−1. A mechanistic study revealed that the m-TS-1 catalysts accepted the migrated OOH− and formed a Ti-OOH intermediate, which played a key role in relaying the tandem reactions for an efficient propylene epoxidation reaction. Techno-economic analysis and life-cycle assessment revealed favorable figures for the proposed process compared to the conventional process.
研究领域:
化学工程
·
催化科学
·
环境科学
✓ 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）