Nature Communications
·
2025
·Vol. 16
·期 1
·1-11
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IF 15.7
Yi Kexin,Li Chao,Hu Shaogang,Yuan Xiayu,Logan Bruce E.,Yang Wulin
Hydrogen peroxide (H 2 O 2 ) can be sustainably synthesized through the electrochemical oxygen reduction reaction in a dual-chamber water electrolyzer separated by expensive ion exchange (IX) membranes. The development of an IX membrane-free electrolyzer has been limited by direct anodic degradation of the produced H 2 O 2 . Here, we devise a bubble shielding strategy by using a low-cost polytetrafluoroethylene hydrophobic porous layer (HPL) on the anode that enables numerous sites for anodically generated oxygen bubbles and significantly suppresses H 2 O 2 degradation in the electrolyte. The H 2 O 2 production increases by ~600% compared to that using non-bubble shielded anode. A high H 2 O 2 concentration of 10.05 ± 0.05 g L −1 at 40 mA cm −2 can be obtained with both HPL-coated anode and cathode. A solar-driven disinfection device equipped with HPL-coated electrodes achieves >99.9% E. coli inactivation within 60 min. This innovative approach for achieving high electrochemical H 2 O 2 concentrations in IX membrane-free electrolyzers more generally provides insights for fine tuning three-phase interfaces and could be applicable to other reactions pathways in electrochemical applications.
研究领域:
环境科学
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化学工程
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生物学
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产品关联
DOI
PubMed
高影响因子
IONICS
·
2022
·Vol. 28
·期 9
·4321-4329
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IF 2.961
Zhang Jin-Zhong,Wu Shuai,Shen Fengxia,Song Wenkang,Hua Yaxin,Wu Zhenyu,Zhang Xiao-Gang,Shi Jin
A novel gas diffusion electrode (GDE) electrolyzer has been constructed to convert CO 2 into CO, with chlorine (Cl 2 ) and sodium carbonate (Na 2 CO 3 ) produced as the by-products. Using this method, the product value yielded from CO 2 electrolysis can be increased substantially. In contrast to the conventional GDE electrolyzer, we use a cation-exchange membrane as the diaphragm to separate the cathode from the anode compartment, and use NaCl aqueous solution as the anolyte. During the electrolysis process, CO 2 is reduced to CO on the cathode, with CO 3 2− generated accompanied with CO formation. On the anode, Cl − is oxidized to Cl 2 . Na + in the anode chamber transfers through the cation-exchange membrane, and migrates into the catholyte. Thus, Na 2 CO 3 can be obtained owing to the co-existing of Na + and CO 3 2− in the catholyte. Using this method, CO 3 2− penetrating through the anion-membrane can be avoided. This problem has been considered as the crucial obstacle that impedes the practical utilization of the conventional GDE electrolyzer. Our designed GDE electrolyzer has a promising application perspective in the phosgene chemical industry.
研究领域:
化学工程
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环境科学
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DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
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2024
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IF 8.4
Shuai Zhang,Xiaofeng Li,Yanqin Yang,Jingde Li,Jifu Zheng,Suobo Zhang
The Development of high-efficiency anion exchange membrane water electrolyzers (AEMWEs) depends on a well-designed anion exchange membrane (AEM) that possesses good mechanical robustness, high alkaline stability, and enhanced ionic conductivity. Herein, we use tetraphenylmethane as a branched monomer to create AEMs with branched structure based upon poly(aryl piperidinium)s. When five molar percentage of tetraphenylmethane is incorporated, the quaternized poly( p -terphenyl-tetraphenylmethane-piperidinium) membrane (QPTTP-5%) exhibits low water swelling ratio (8.53% at 80 °C) and decent mechanical strength (31.95 MPa). Meanwhile, the high microporosity and obvious microphase separation behavior of the as-developed QPTTP-5% membrane engendered by the rigid and tetrahedral tetraphenylmethane branched structure improve hydroxide conductivity, reaching 164.70 mS cm −1 at 80 °C. Moreover, the current density of the AEMWE single cell comes up to 1500 mA cm −2 at 2.2 V and 80 °C with the implementation of QPTTP-5% membrane. This study reveals that the introduction of a rigid and three-dimensional branched structure is conducive to the preparation of high-performance AEMs with microporous structure and low swelling ratio.
研究领域:
材料科学
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化学工程
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DOI
高影响因子
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
·
2024
·Vol. 121
·期 43
·e2414741121
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IF 9.4
Xiaosong Gu,Xuezhen Feng,Songhe Yang,Ranhao Wang,Qiang Zeng,Yangzi Shangguan,Jiaxin Liang,Huiling Zhou,Zhiwei Li,Zhang Lin,Chunmiao Zheng,Zhenghe Xu,Hong Chen
The insatiable demand for lithium in portable energy storage necessitates a sustainable and low-carbon approach to its recovery. Conventional hydrometallurgical and pyrometallurgical methods heavily involve hazardous chemicals and significant CO2 emissions. Herein, by integrating electrode oxidation with electrolyte oxidation, we establish a photovoltaic-driven “dual-oxidation” seawater electrolyzer system for low-carbon footprint and high lithium recovery. A 98.96% lithium leaching rate with 99.60% product purity was demonstrated for lithium recovery from spent LiFePO4 cathode materials. In-depth mechanism studies reveal that the electric field-driven electrode oxidation and in situ generated oxidative electrolyte synergetically contributes to lithium ions leaching via a structural framework elements oxidation and particle corrosion splitting synergy. This dual-oxidation mechanism facilitates rapid and efficient lithium extraction with broad universality, offering significant economic and environmental benefits. Our work showcases a promising strategy for integrating dual oxidation within a photovoltaic-driven seawater electrolyzer, paving the way for low-carbon lithium recovery from diverse solid wastes and minerals within a sustainable circular economy.
研究领域:
材料科学
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环境科学
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能源技术
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产品关联
DOI
PubMed
高影响因子
Chemistry-An Asian Journal
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2023
·Vol. 18
·期 16
·e202300440
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IF 4.1
Wen Sun,Ying Fang,Gaoming Sun,Congfu Dai,Yana Liu,Jiguang Zhang,Yunfeng Zhu,Jun Wang
Graphical A rutile Ru 0.75 Mn 0.25 O 2−δ solid solution oxide with a porous structure and high Ru >4+ proportion has been developed as an efficient electrocatalyst for simultaneously boosting oxygen evolution reaction under acidic and alkaline conditions, outperforming the commercial RuO 2 and many previously reported catalysts. Proton exchange membrane water electrolysers and alkaline exchange membrane water electrolysers for hydrogen production suffer from sluggish kinetics and the limited durability of the electrocatalyst toward oxygen evolution reaction (OER). Herein, a rutile Ru 0.75 Mn 0.25 O 2−δ solid solution oxide featured with a hierarchical porous structure has been developed as an efficient OER electrocatalyst in both acidic and alkaline electrolyte. Specifically, compared with commercial RuO 2 , the catalyst displays a superior reaction kinetics with small Tafel slope of 54.6 mV dec −1 in 0.5 M H 2 SO 4 , thus allowing a low overpotential of 237 and 327 mV to achieve the current density of 10 and 100 mA cm −2 , respectively, which is attributed to the enhanced electrochemically active surface area from the porous structure and the increased intrinsic activity owing to the regulated Ru >4+ proportion with Mn incorporation. Additionally, the sacrificial dissolution of Mn relieves the leaching of active Ru species, leading to the extended OER durability. Besides, the Ru 0.75 Mn 0.25 O 2−δ catalyst also shows a highly improved OER performance in alkaline electrolyte, rendering it a versatile catalyst for water splitting.
研究领域:
材料科学
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电化学
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能源材料
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催化
✓ 已验证
DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
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2022
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IF 10.53
Tao Jiang,Chenxi Wang,Tao Wang,Xuechao Wang,Xiaojuan Wang,Xueliang Li,Yunsheng Ding,Haibing Wei
Anion exchange membranes (AEMs) are a core component for energy conversion technologies such as fuel cells and water electrolyzers. Unfortunately, the functional cations in AEM often suffer from inferior durability in caustic media, especially at elevated temperatures or highly concentrated alkaline solutions. Therefore, the exploitation of novel cations that can endure highly alkaline environments while with synthetic feasibility and good ion conducting property is desired. Herein, a simple and easily available pyrazolium cation was evaluated and was alkaline stable in 5 M NaOH (aq) at 80 °C for at least 240 h, which is substantially stable than its structural isomer, imidazolium. The alkaline stability of pyrazolium was rationalized through analyses of the degradation energy barriers calculated by density functional theory. The excellent alkaline stability of pyrazolium cation encouraged the fabrication of AEMs functionalizing with pyrazolium head group anchored to poly(arylene alkylene) architecture. In contrast to imidazolium-based counterpart, pyrazolium cation enable the AEM with higher base stability, retaining ～80% of its initial conductivity after a 1000-h treatment in 1 M NaOH (aq) at 80 °C. Moreover, the AEM based on pyrazolium showed a high hydroxide ion conductivity up to 120 mS cm −1 at 80 °C and a high peak power density of 502 mW cm −2 after assembled into a H 2 –O 2 fuel cell device.
研究领域:
材料科学
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能源转换技术
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电化学
✓ 已验证
DOI
高影响因子
Chem Catalysis
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2023
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IF 9.4
Qiming Chen,Ning Gong,Qicheng Zhang,Wenchao Peng,Yang Li,Fengbao Zhang,Xiaobin Fan
Facet engineering is frequently employed to give catalysts the desired surface atom configurations and morphologies for enhanced catalytic performances. However, constructing single-crystal bimetallic hydroxides and understanding their facet effects are still challenging. Here, by adjusting the dissociated OH − concentration, 2D nanosheets (NSs) exposing (020) facet (CoCu (020) NS) and 1D nanorods mainly exposing (031) facet of single-crystal bimetallic kolwezite are precisely synthesized. CoCu (020) NS shows superior performances in alkaline hydrogen evolution and anion exchange membrane water electrolyzer. Combining characterizations and theoretical calculations shows that CoCu (020) NS exhibits a local geometric structure with low coordination number and an electron structure with appropriate d-band center level and charge density of active sites, both of which are strongly correlated with the adsorption properties of H 2 O and intermediates. This work might pave the way for development of single-crystal bimetallic hydroxides and further applications of facet engineering in electrocatalysis.
研究领域:
材料科学
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电化学
✓ 已验证
DOI
高影响因子
Progress in Natural Science-Materials International
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2024
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IF 4.8
Xue Deng,Siyang Wang,Qianqian Ren,Xintong Yan,Wenbo Zhao,Jianzhong Cui,Shi Hu
Energy transition towards net-zero society calls for utilization of renewable power to drive CO 2 conversion in an efficient electrochemical way. The development of a commercial CO 2 electrolyzer with positive tech-eco effect calls for active and durable electrocatalysts. High-loading gold on carbon (Au/C) with reduced particle size is the prerequisite for the highly-selective and highly energy-efficient CO production in such a CO 2 electrolyzer, but a scalable synthetic method is missing. With combined control of ligand, substrate and pH value, Au/C catalysts with particle size within 5 nm and metal loading of 40 wt% and 60 wt% are synthesized on low and high surface-area carbon, respectively. We also provide a thorough investigation of the effect of the ligand type, surface charge of gold nanoparticles (Au NPs) and surface area of carbon substrate on the loading limit of Au/C.
研究领域:
材料科学
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电化学
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可再生能源
✓ 已验证
产品关联
DOI
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-9
·
IF 14.7
Zhou Chenhui,Li Lu,Dong Zhaoqi,Lv Fan,Guo Hongyu,Wang Kai,Li Menggang,Qian Zhengyi,Ye Na,Lin Zheng,Luo Mingchuan,Guo Shaojun
Ruthenium (Ru) is widely recognized as a low-cost alternative to iridium as anode electrocatalyst in proton-exchange membrane water electrolyzers (PEMWE). However, the reported Ru-based catalysts usually only operate within tens of hours in PEMWE because of their intrinsically high reactivity of lattice oxygen that leads to irrepressible Ru leaching and structural collapse. Herein, we report a design concept by employing large-sized and acid-resistant lattice lead (Pb) as a second element to induce a pinning effect for effectively narrowing the moving channels of oxygen atoms, thereby lowering the reactivity of lattice oxygen in Ru oxides. The Pb-RuO 2 catalyst presents a low overpotential of 188 ± 2 mV at 10 mA cm −2 and can sustain for over 1100 h in an acid medium with a negligible degradation rate of 19 μV h −1 . Particularly, the Pb-RuO 2 -based PEMWE can operate for more than 250 h at 500 mA cm −2 with a low degradation rate of only 17 μV h −1 . Experimental and theoretical calculation results reveal that Ru-O covalency is reduced due to the unique 6 s −2 p −4 d orbital hybridization, which increases the loss energy of lattice oxygen and suppresses the over-oxidation of Ru for improved long-term stability in PEMWE.
研究领域:
电化学
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材料科学
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催化
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能源存储与转换
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产品关联
DOI
PubMed
高影响因子
CHEMISTRY-A EUROPEAN JOURNAL
·
2022
·Vol. 29
·期 5
·e202202858
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IF 5.02
Yongsheng Wang,Xinyu Wang,Hailong Wei,Junling Huang,Likun Yin,Wei Zhu,Zhongbin Zhuang
Graphical This work reports the homogeneous incorporation of Co into the FeP host to promote both activity and stability of HER for the PEMWE application and demonstrates the probable origin of the high performance by ex situ experiments. Metal phosphides are promising noble metal-free electrocatalysts for hydrogen evolution reaction (HER), but they usually suffer from inferior stability and thus are far from the device applications. We reported a facile and controllable synthetic method to prepare metal-incorporated M-FeP nanoparticles (M=Cr, Mn, Co, Fe, Ni, Cu, and Mo) with the guide of the density functional theory (DFT). The evaluated HER activity sequence was consistent with the DFT predictions, and cobalt was revealed to be the appropriate dopant. With the optimization of the Co/Fe ratio, the Fe 0.67 Co 0.33 P/C only required overpotentials of 67 mV and 129 mV to obtain the cathodic current density of 10 and 100 mA cm −2, respectively. It maintained the initial activity in the 10 h stability test, surpassing the other Co-FeP/C catalysts. Ex situ experiments demonstrated that the decreased element leaching and the increased surface phosphide content contributed to the high stability of the Fe 0.67 Co 0.33 P/C. A proton exchange membrane water electrolyzer was assembled using the Fe 0.67 Co 0.33 P/C as the cathodic catalyst. It showed a current density of 0.8 A cm −2 at the applied voltage of 2.0 V and retained the initial activity in the 1000 cycles’ stability test, suggesting the potential application of the catalysts.
研究领域:
电化学
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材料科学
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催化
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可再生能源
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Boyuan Liu,Peng Zhao,Zongdeng Wu,Cai Liu,Haiyan Jing,Juanjuan Song,Keren Lu,Wu Lei,Qingli Hao
The exploration of bifunctional catalyst with economic, durable, and efficient performance plays a crucial role to boost both hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) in overall water splitting. Herein, we report a feasible strategy to design effective heterostructure between CoP and Ti 3 C 2 T x MXene (denoted as CoP/Ti 3 C 2 T x ). This approach allows for the growth of CoP nanoparticles with uniform size of 5 nm on the Ti 3 C 2 T x MXene, further enhancing the water electrolysis efficiency. The CoP/Ti 3 C 2 T x bifunctional catalyst demonstrates an exceptional HER activity with a satisfactory overpotential of 103 mV at 10 mA cm −2 , and also can drive 10 mA cm −2 for OER with the overpotential of 312 mV in 1.0 M KOH. Moreover, the CoP/Ti 3 C 2 T x -based electrolyzer exhibits high electrochemical stability for 24 h with a low required voltage of 1.66 V at 10 mA cm −2 . The density functional theory (DFT) calculations reveal that the introduction of Ti 3 C 2 T x MXene significantly adjusts d-band center towards Fermi level and expand total density of states, resulting in great electrical conductivity, enhanced water adsorption, and activation. This study provides an available mode for effective design and construction of non-noble-metal-based dual-functional catalyst toward practical energy conversion.
研究领域:
材料科学
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电化学
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能量转换
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产品关联
DOI
PubMed
高影响因子
ACS Applied Energy Materials
·
2024
·
IF 5.4
Yue Yang,Nanhui Li,Jianghao Wang,Wei Zhao,Hao Bin Wu
Gas diffusion electrodes (GDEs) show great potential to improve the current densities of the industrial electrochemical carbon dioxide reduction reaction (eCO2RR). The triple-phase boundary (TPB) in GDEs is the key for promoted reaction kinetics, yet such a reaction interface typically suffers from rapid degradation due to electrolyte flooding and salt precipitation. Herein, we demonstrate that a GDE modified with liquid perfluorocarbon (PFC) would notably prolong the lifespan of the GDE with a Bi catalyst in flow-cell electrolyzers. PFC with superhydrophobicity and high CO2 solubility would construct a liquid–solid–liquid reaction interface that prevents the intrusion of electrolytes into the microporous layer (MPL) without hampering the mass transport of CO2. Our work demonstrates an effective strategy to construct a robust and efficient electrochemical reaction interface for the eCO2RR with improved stability for potential industrial applications.
研究领域:
电化学
·
材料科学
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可持续能源
✓ 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）