FUEL
·
2025
·
IF 7.5
Jiaojiao Chen,Yu Chen,Ke Bai,Jingyun Liu,Zewei Bao,Zeyi Xiao,Senqing Fan
To enhance mass transfer in hydrogen production from water electrolysis coupled with ethanol oxidation, a membrane electrolyzer combining flow-through and fed-batch operation was developed. The optimized Co 0.1 Ni 0.9 (OH) 2 /Ni foam electrode was used for ethanol oxidation, with a current density of 200 mA cm −2 at 1.383 V vs. RHE and a Tafel slope of 39.5 mV dec -1 . Employing this electrode as the anode, the mass transfer coefficient ( k m ) in the flow-through electrolyzer was 7.0 × 10 -6 m s −1 under the conditions of electrolyte flow velocity at 0.06 m s −1 , ethanol concentration at 0.2 M and KOH concentration at 6 M, which was 49 % higher than that in the flow-by electrolyzer. This enhancement in k m directly translated to an increase in the mass transfer limiting current density ( i L , from 194 mA cm −2 to 289 mA cm −2 ), significantly higher reaction rate. Both k m and i L would be increased with the increase of electrolyte circulation rates. An analysis of the relationship between intrinsic electrochemical current density and i L showed that the ethanol oxidation process is maintained at or near the i L , which improved current efficiency and product yield. A fed-batch strategy, regulating ethanol concentration around 0.2 M, enabled sustained co-production of acetic acid and hydrogen at current densities of 289 mA cm −2 , with a production rate of 18.54mol h −1 m −2 (electrode) and 43.75 mol h −1 m −2 (electrode) respectively, with an anodic Faradaic efficiency of 92 %. The hydrogen production energy consumption was 3.85 kWh Nm −3 under this condition in flow-through electrolyzer.
研究领域:
化学工程
·
能源科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2021
·
IF 4.464
Yajian Duan,Chaojuan Li,Yaxin Hua,Shuai Wu,Yaqing Guo,Xiaogang Zhang,Yuqi Hu,Bin Yang,Yongnian Dai,Jin Shi
A novel membrane electrolysis cell has been designed to convert CO 2 into CO in organic electrolyte, with Cl 2 produced on the anode from NaCl oxidation in aqueous solution. The obtained CO and Cl 2 can be used as the feedstock to produce phosgene. Phosgene is a widely used acylating agent in a chemical industry, which can be used as feedstock to produce numerous high-value chemicals. Through this route, CO 2 can be converted into useful chemical, with huge economic profits created in this process. Our experiment results demonstrate that CO 2 can be efficiently converted into CO in our designed electrolyzer, and NaCl can be efficiently oxidized to Cl 2 . During long-term electrolysis process, NaHCO 3 is generated and accumulated between the membrane and the cathode. This phenomenon provides clear evidence for us to better understand the mechanism of CO 2 electro-reduction in organic electrolyte.
研究领域:
化学工程
·
电化学
·
环境科学
✓ 已验证
DOI
高影响因子
FUEL
·
2025
·
IF 7.5
Shiqing Zhang,Shaokai Ma,Zihao Wang,Zihang Cao,Fang Liu,Ying Li,Xuewen Xu,Yuanhui Ma,Yanming Xue,Chengchun Tang,Jun Zhang
The development of cost-effective, highly efficient, and stable electrocatalysts for the acidic hydrogen evolution reaction (HER) is essential for advancing clean and renewable hydrogen energy technologies. This is particularly critical for proton exchange membrane (PEM) electrolyzers powered by renewable energy sources. Among various candidates, cobalt-based phosphide (CoP) has emerged as a promising catalyst for the HER in acidic media, owing to the synergistic interaction between Co and P, as well as its inherent stability. Despite significant efforts to enhance its catalytic activity, the critical issue of stability has often been overlooked. Herein, sulfur (S), which has a higher electronegativity than P, is selectively incorporated into CoP nanowire arrays through a simple vulcanization method. This strategy aims to enhance stability without altering catalytic activity. The optimized S-CoP/CC electrocatalyst shows an overpotential of 96 mV at 10 mA cm −2 in acid electrolyte, showing a slight improvement over the initial CoP/CC (114 mV). Remarkably, it shows exceptional durability, maintaining excellent stability over 150 h of testing in acid solution. The incorporation of sulfur serves a dual role: it enhances electronic conductivity and increases the electrochemical surface area, thereby improving catalytic activity, while simultaneously strengthening the CoP bond energy, leading to outstanding acid stability. Furthermore, when employed as the cathode in a PEM electrolyzer, S-CoP/CC achieves a current density of 500 mA cm −2 at 1.70 V, demonstrating excellent stability over 140 h at 60 °C. Our findings present a new approach for enhancing both the stability and activity of acidic HER by incorporating higher-electronegativity anions into the CoP lattice. This strategy is applicable not only to Co-based phosphides but also to other non-precious metal-based transition metal compounds, paving the way for the development of high-performance PEM electrolyzers.
研究领域:
材料科学
·
能源技术
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
Advanced Energy Materials
·
2021
·Vol. 11
·期 48
·2102883
·
IF 29.368
Jing He,Xin Zhou,Ping Xu,Jianmin Sun
Developing high-performance electrocatalysts to catalyze water splitting for the generation of sustainable hydrogen remains a challenge in proton exchange membrane (PEM) electrolyzers. However, the only applicable IrO x in PEM electrolyzers for oxygen evolution reaction (OER) with a multiproton-coupled process, requires a higher standard due to the weak oxygen bonding on Ir sites, which causes high overpotential and poor stability under oxidative and acidic conditions. Herein, the intermetallic Ru 1 Ir 1 O x is synthesized through incorporation of Ru into IrO x , which exhibits a record overpotential of 204 mV (10 mA cm −2 geo ) and excellent stability of 110 h (100 mA cm −2 geo ) with a high stability number (1.13 × 10 6 ) toward the acidic OER. Through fine characterizations, Ir sites with lower than +4 valence state are observed due to charge redistribution, in turn enhancing the acidic OER performance. Theoretical calculations reveal that incorporation of Ru effectively moves the Fermi level to the Ir 5d band center, thus enhancing the adsorption of oxygen intermediates and decreasing the energy barrier of the potential-determining step from 1.02 to 0.65 eV. The decreased valence states of Ir and enhanced valence state of Ru due to the charge redistribution significantly tunes the electronic structure of Ir sites, thereby drastically enhancing the OER 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 Cleaner Production
·
2023
·
IF 11.1
Songlin Liu,Zhixing Wang,Ding Wang,Huajun Guo,Guochun Yan,Guangchao Li,Wenjie Peng,Xinhai Li,Jiexi Wang
In this paper, a material-oriented metallurgical electrolysis strategy, which is of such characteristics as short process, easy procedure, and nonpollution, is proposed to treat sodium sulfate wastewater and simultaneously prepare high value-added cathode material LiNi 1/3 Co 1/3 Mn 1/3 O 2 for lithium-ion batteries. The strategy is divided into two parts. First, the Ni 1/3 Co 1/3 Mn 1/3 (OH) 2 precursor is obtained by double membrane electrolyzing a mixed solution of Na 2 SO 4 , NiSO 4 , CoSO 4 , and MnSO 4 under the optimum electrolysis conditions (60 °C, 1.0 A). Furthermore, LiNi 1/3 Co 1/3 Mn 1/3 O 2 cathode is obtained through solid-sintering desulfurization . The change of sulfur content in the process and its effect on the morphology and electrochemical properties of the materials are investigated. Under optimum desulfurization conditions, the LiNi 1/3 Co 1/3 Mn 1/3 O 2 electrode delivers a high initial specific discharge capacity of 195.0 mAh·g −1 and a satisfying capacity retention of 85.0% after 120 cycles at 0.1 C in 2.5–4.5 V. This innovative strategy can realize the comprehensive utilization of sodium sulfate wastewater for preparation of Ni, Co, Mn-contained layered cathode materials.
研究领域:
冶金工程
·
材料科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Xiaohui Zhao,Xinmin Wei,Mengxue He,Haoran Cheng,Jiapeng Hu,Yanzhi Zhang,Yongze Qin,Yang Peng,Zhao Deng
Membrane electrolytes are key to constructing planar energy storage devices of low thickness and high flexibility, requesting simultaneous optimization of ionic conductivity and mechanical stability. Herein, aqueous phase electrospinning (APE) was implemented to co-spin polyvinyl alcohol and pullulan polysaccharide for fabricating crosslinked fibrous membrane electrolytes. While the hydroxyl-rich polymeric backbone grafted with quaternary ammonium endows a strong hydrogen-bonding network affording a large ionic conductivity of 30.2 mS cm −1 , the cellulose-braced fibrous structure manifests a high tensile strength of 4.6 MPa. What’s more, the porous structure of the membrane electrolyte with enhanced charge mobility and uniformity helps to guide homogeneous Zn plating/stripping with suppressed dendrite growth. As a result, the assembled ultrathin flexible ZAB delivers a superb round-trip energy efficiency of 59.8 %, a maximum power density of 102 mW cm −2 and a long-term cycling stability over 100 h at 5 mA cm −2 . By innovating the concept and methodology of aqueous fibrous membrane electrolytes, this study opens up a new chapter on the development of solid electrolytes in aqueous battery systems for powering wearable electronics.
研究领域:
材料科学
·
能源存储
·
柔性电子
✓ 已验证
DOI
高影响因子
Advanced Sustainable Systems
·
2024
·
IF 6.5
Qi Ding,Linfeng Xie,Zijie Lin,Zhuhuang Qin,Yunan Li,Qing Li
The low activity of ruthenium dioxide (RuO 2 ) and the rapid dissolution of the ruthenium (Ru) site during acid oxygen evolution reaction (OER) at high current density restricts its application in proton exchange membrane (PEM) electrolyzers. In this work, a series of rare-earth (RE) elements doped RuO 2 nanorods is developed as high-performance OER electrocatalysts. X-ray absorption spectroscopy suggests that RE doping regulates the local coordination environment around Ru sites, lowers the valance of Ru, and shortens the Ru─O─Ru(M) bond length, which enhances structural stability. Among the RE-RuO 2 samples, Sm-RuO 2 exhibits remarkable performance with a low overpotential of 283 mV to reach 100 mA cm −2 and maintained stability for over 140 h at 10 mA cm −2 . Moreover, the PEM electrolyzer using Sm-RuO 2 as the anode can be stably operated at 500 mA cm −2 for 15 h. Electrochemical analysis, X-ray photoelectron spectroscopy, and in situ Raman spectroscopy show that Sm doping lowers the d -band center, reduces the adsorption energy of O intermediates to enhance the OER activity, and restrains excessive oxidation of Ru sites while stabilizing lattice oxygen during the OER process, thereby enhancing OER stability. This work offers valuable insights into improving the stability of metal oxide catalysts in acidic electrolytes.
研究领域:
材料科学
·
电化学
·
催化科学
✓ 已验证
产品关联
DOI
高影响因子
Matter
·
2025
·
IF 17.5
Tingting Zhai,Xutao Gao,Hao Wang,Yaojia Cheng,Jingchi Gao,Jie Pan,Edmund C.M. Tse,Congxiao Shang,Zhengxiao Guo
Activity and stability are often inversely entwined in catalysis, especially for the water oxidation reaction (WOR) to generate hydrogen under acidic media. Here, we show that an ionic-mismatch-induced semi-crystalline Y 0.3 Ru 0.7 O 2 gives rise to exceptionally active and stable WOR performance. The mismatched ionic radii and valences between Y 3+ and Ru 4+ leads to a strongly bonded hybrid nanostructure of ultra-fine crystalline and amorphous domains. The short-range ordered structure also leads to a reduced adjacent distance, which facilitates a more efficient and stable dual-site coupling mechanism with an extremely low overpotential of 170 mV at 10 mA cm −2 and prolonged stability over 300 h in an acidic electrolyte. A proton-exchange-membrane (PEM) water electrolyzer loaded with the catalyst shows an outstanding performance with only 1.64 V to reach 1 A cm −2 and stable operation at 0.5 A cm −2 over 300 h, demonstrating its outstanding potential for practical applications in PEM electrolysis.
研究领域:
材料科学
·
催化化学
·
能源科学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Yue Shi,Jiawei Fei,Hongdong Li,Caixia Li,Tianrong Zhan,Jianping Lai,Lei Wang
Amorphous metallene is a prospective catalyst due to disordered atomic arrangement and abundant defects/edges. However, challenges persist in preparing amorphous metallene with atomic interface, primarily due to thermodynamic impediment of unconventional phase and difficulty in precise controlling of atomic interface. Here, we synthesized a new class of amorphous RuGa metallene (A-RuGa metallene) with abundant atomic interface by introducing trace atomic-dispersed Ga. The atomic interface between Ga-coordinated Ru and Ru 0 achieves monometallic synergism during alkaline hydrogen evolution reaction. The turnover frequency value of A-RuGa 0.06 metallene reaches 67 s −1 at −0.1 V vs. RHE. Meanwhile, the mass activity of A-RuGa 0.06 metallene in anion exchange membrane electrolyzer reaches 5.2 A mg Ru −1 at 2.0 V, firstly surpassing commercial Pt/C (1.0 A mg Pt −1 ). The trace atomic dispersed Ga could change the local valence state of monometallic Ru, thus promoting water adsorption and dissociation, optimizing H* adsorption and accelerating H* transport at the atomic level.
研究领域:
材料科学
·
电催化
·
能源转换
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2024
·
IF 8.1
Xingzhao Wang,Jian Che,Tingyong Wang,Fengqi Xu,Dongxia Duan
Low intrinsic electrocatalytic activity and inferior conductivity limit the application of Ni/NC in acidic electrocatalytic hydrogen evolution reaction (HER). Herein, we prepared nitrogen-doped carbon nanosheet confined PtNi alloy electrocatalysts (PtNi/NC-10) using PtCl 6 2− electrostatic adsorption coupling melamine pyrolysis nitriding strategy. PtNi alloying was confirmed by the crystallinity decrease and lattice expansion of Ni/NC. The alloying and confinement effect of Metal-Organic Frameworks (MOFs) suppresses the oxidation and agglomeration of metal nanoparticles during pyrolysis, thus significantly reducing particle size, increasing specific surface area, and promoting the exposure of active sites. The strong electronic interaction between Pt and Ni optimizeds the surface charge distribution, enhancing the adsorption of H species on electron-rich Pt sites, thereby improving reaction kinetics. In addition, PtNi alloying improves the conductivity of the material, accelerating charge transfer and proton transport. Consequently, the prepared PtNi/NC-10 exhibits superior HER performance than Ni/NC in 0.5 M H 2 SO 4 solution, even comparable to commercial 20 wt % Pt/C, with the overpotentials of 35 mV at 0.01 A cm −2 . Furthermore, the electrocatalysts assembled PtNi/NC-10-CP‖RuO 2 -TFF proton exchange membrane (PEM) electrolyzer only requires 2.32 V cell voltage to achieve 1 A cm −2 , presenting practical application prospects. Our work provides a novel idea for designing efficient and stable MOFs confined to alloy-based HER electrocatalysts.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
Nature Communications
·
2023
·Vol. 14
·期 1
·1-14
·
IF 16.6
Shi Zhaoping,Li Ji,Wang Yibo,Liu Shiwei,Zhu Jianbing,Yang Jiahao,Wang Xian,Ni Jing,Jiang Zheng,Zhang Lijuan,Wang Ying,Liu Changpeng,Xing Wei,Ge Junjie
The poor stability of Ru-based acidic oxygen evolution (OER) electrocatalysts has greatly hampered their application in polymer electrolyte membrane electrolyzers (PEMWEs). Traditional understanding of performance degradation centered on influence of bias fails in describing the stability trend, calling for deep dive into the essential origin of inactivation. Here we uncover the decisive role of reaction route (including catalytic mechanism and intermediates binding strength) on operational stability of Ru-based catalysts. Using MRuO x (M = Ce 4+ , Sn 4+ , Ru 4+ , Cr 4+ ) solid solution as structure model, we find the reaction route, thereby stability, can be customized by controlling the Ru charge. The screened SnRuO x thus exhibits orders of magnitude lifespan extension. A scalable PEMWE single cell using SnRuO x anode conveys an ever-smallest degradation rate of 53 μV h −1 during a 1300 h operation at 1 A cm −2 .
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
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Yuan Yang,Dongfang Chen,Lei Wang,Song Hu,Pucheng Pei,Xiaoming Xu
Proton exchange membrane water electrolyzer (PEMWE) coupled with renewable energy is an ideal way to produce green hydrogen. However, the high load of precious metal catalysts and the requirement of catalyst durability in acidic environment restrict the large-scale application of PEM electrolyzers. Herein, an IrCo alloy electrocatalyst supported on metal titanium nitride (TiN) is synthesized, which has excellent acid oxygen evolution reaction (OER) activity and durability. The electrocatalyst exhibits a low overpotential of 246 mV@10 mA cm −2 and a higher mass activity of 0.84 A mg Ir −1 at 1.53 V in 0.5 M H 2 SO 4 . After stable operation for more than 220 h at 10 mA cm −2 , the degradation rate is negligible. When used as an anode catalyst (0.2 mg Ir cm −2 ) for the PEM electrolyzer, only 1.78 V is needed to reach 1.0 A cm −2 . The structure characterization and theoretical calculation (DFT) show that there is a strong electron coupling between TiN support and IrCo alloy. This unique effect regulates the d-band center of IrCo@TiN and optimizes the adsorption energy of the oxygen-containing intermediates, which effectively reduces the energy barrier of *O forming *OOH in the rate-determining step of OER catalytic reaction.
研究领域:
材料科学
·
电化学
·
可再生能源
✓ 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）