ADVANCED MATERIALS
·
2024
·Vol. 36
·期 30
·2401694
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IF 27.4
Yin Zhu,Yanxu Chen,Yafei Feng,Xiangmin Meng,Jing Xia,Genqiang Zhang
Hydrazine oxidation-assisted water splitting is a critical technology to tackle the high energy consumption in large-scale H 2 production. Ru-based electrocatalysts hold promise for synergetic hydrogen reduction (HER) and hydrazine oxidation (HzOR) catalysis but are hindered by excessive superficial adsorption of reactant intermediate. Herein, this work designs Ru cluster anchoring on NiFe-LDH (denoted as Ru c /NiFe-LDH), which effectively enhances the intermediate adsorption capacity of Ru by constructing Ru─O─Ni/Fe bridges. Notably, it achieves an industrial current density of 1 A cm −2 at an unprecedentedly low voltage of 0.43 V, saving 3.94 kWh m −3 H2 in energy, and exhibits remarkable stability over 120 h at a high current density of 5 A cm −2 . Advanced characterizations and theoretical calculation reveal that the presence of Ru─O─Ni/Fe bridges widens the d-band width (W d ) of the Ru cluster, leading to a lower d-band center and higher electron occupation on antibonding orbitals, thereby facilitating moderate adsorption energy and enhanced catalytic activity of Ru.
研究领域:
材料科学
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电化学
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能源技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2024
·
IF 15.7
Jieting Ding,Hao-Fan Wang,Kui Shen,Xiaoming Wei,Liyu Chen,Yingwei Li
The applications of metal-organic frameworks (MOFs) in electrocatalysis are limited by the perfect crystalline nature with insufficient coordinatively unsaturated sites and low electronic conductivity. Here, we report an electrosynthesis method to induce rapid assembly of amorphous MOFs on carbon cloth (denoted as a MnFc’/CC), achieving the amorphization of MOFs with rich active sites and high electronic conductivity. The long-range disordered structure of a MnFc’/CC forms a large number of oxygen vacancies to modify the coordination and electronic structures of Mn sites. In the electrocatalytic hydrazine oxidation reaction (HzOR), the a MnFc’/CC electrocatalyst exhibits superior activity to its crystalline MOF counterparts. Density functional theory calculations reveal that the unsaturated Mn centers present in aMnFc’/CC facilitate efficient electron transfer while simultaneously lowering the free energy of the rate-determining step in the HzOR 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 ALLOYS AND COMPOUNDS
·
2024
·
IF 5.8
Xiang Ji,Yaodong Yu,Aixin Ma,Yujia Guan,Hongdong Li,Jianping Lai,Lei Wang
Nitrate (NO 3 - ) and hydrazine (N 2 H 4 ) are common nitrogen pollutants in groundwater. The electrochemical method can be used to synthesize the added product urea while treating N-pollution. Therefore, the development of sufficiently efficient electrosynthesis urea systems and efficient electrocatalysts is of great significance, but also challenging. In this paper, CuNi alloy nanosheets (Cu x Ni y /CF) on copper foam surface were synthesized by electrodeposition, and C-N coupled hydrazine oxidation (HzOR) system was constructed by proton exchange membrane (PEM). Cu and Ni in CuNi alloy act as double active sites and react with C-N coupling reaction and HzOR respectively. At −0.5 V potential, the Faraday efficiency of Cu 8 Ni 2 /CF for C-N coupling reaction is 51.66 %, and the urea yield is 254.09 μg h −1 cm −2 . At the same time, HzOR with low thermodynamic oxidation potential can quickly produce excess H + to supply protons to the cathode for C-N coupling reaction, thus significantly promoting the forward C-N coupling reaction. Cu 1 Ni 9 /CF also showed significant activity in the oxidation reaction of N 2 H 4 in KOH electrolyte. Therefore, we assembled a Cu 1 Ni 9 (+) || Cu 8 Ni 2 (-) electrolytic cell, which only needs 0.23 V working voltage up to 150 mA cm −2 , and can convert NO 3 - and CO 2 to urea at a power consumption of 5.09 kWh kg −1 while converting N 2 H 4 . Energy saving 37.6 % compared to conventional C-N coupled OER electrolytic system (about 8.16 kWh kg −1 urea). It can greatly reduce the cost of urea production, make the price of fertilizer and chemical raw materials more competitive, and promote the development of agriculture and chemical industry while reducing greenhouse gas emissions and nitrogen pollutants in the ecological environment. This study reports a promising and effective strategy for the synthesis of urea and treatment of N contaminants at a small operating voltage.
研究领域:
环境科学
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材料科学
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化学工程
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产品关联
DOI
高影响因子
DALTON TRANSACTIONS
·
2024
·Vol. 53
·期 10
·4574-4579
·
IF 3.5
Jinxing Hou,Kaifeng Mei,Tongtong Jiang,Xinxin Yu,Mingzai Wu
Hydrazine-assisted electrochemical water splitting is an important avenue toward low cost and sustainable hydrogen production, which can significantly reduce the voltage of electrochemical water splitting. Herein, we took a simple approach to fabricate NiFeP nanosheet arrays on nickel foam (NiFeP/NF), which exhibit superior electrocatalytic activity for the hydrogen evolution reaction (HER) and the hydrazine oxidation reaction (HzOR). Our investigations revealed that the excellent electrocatalytic activity of NiFeP/NF mainly arises from the bimetallic synergistic effect, abundant electrocatalytically active sites facilitated by the porous nanosheet morphology, high intrinsic conductivity of NiFeP/NF and strong NiFeP–NF adhesion. We assembled a hydrazine-boosted electrochemical water splitting cell using NiFeP/NF as a bifunctional catalyst for both electrodes, and the overall hydrazine splitting (OHzS) exhibits a considerably low overpotential (100 mV at 10 mA cm−2), and is stable for 40 h continuous electrolysis in a 1 M KOH + 0.5 M N2H4 electrolyte. When it is applied to hydrogen production by seawater electrolysis, its catalytic activity shows strong tolerance. This work provides a promising approach for low cost, high-efficiency and stable hydrogen production based on hydrazine-assisted electrolytic seawater splitting for future applications.
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
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Jiachen Li,Cong Zhang,Chi Zhang,Huijun Ma,Yong Yang,Zhaoqi Guo,Yaoyu Wang,Haixia Ma
Replacing sluggish oxygen evolution reaction (OER) by hydrazine oxidation reaction (HzOR) is an energy-saving approach to assist alkaline overall water splitting (OWS). However, it is still at the infant stage as the unsatisfactory of the design strategies for bifunctional catalysts toward both HzOR and hydrogen evolution, which leads to high working potential compared to the theoretical value. Here, for the first time, we report a galvanostatic immobilization of ruthenium single atoms (Ru SAs) into the oxygen vacancy of urchin-like tungsten trioxide (Vo-WO 3 ) and show low overpotentials of 17, 34, and 64 mV at –10 mA cm –2 under acid, alkaline, and neutral H 2 evolution, respectively. As an efficient bifunctional catalyst, the Vo-WO 3 /Ru SAs is firstly introduced to HzOR and achieves low working potential of –58 mV at 10 mA cm –2 . The HzOR-assisted OWS also delivers an ultralow cell voltage of only 25 mV at 10 mA cm –2 in alkaline medium, which is far beyond the platinum and most of the state-of-the-art catalysts. Additionally, this coupled system can also be well performed under neutral condition, realizing a cell voltage of only 137 mV at 10 mA cm –2 . The excellent pH-universal HzOR-assisted OWS activity is attributed to the particular electronic configuration between Ru SAs and WO 3 , the immobilization of Ru SAs in WO 3 could induce electron redistribution and optimize free energy of hydrogen adsorption in hydrogen evolution, while the isolation of Ru SAs also leads to the electropositivity of W sites and tends to accelerate the oxidation of hydrazine.
研究领域:
材料科学
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催化化学
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能源科学
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产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2024
·
IF 5.8
Xia Wei,Tianyao Wang,Hongbin Dai,Song Li
The hydrazine oxidation reaction (HzOR) plays a critical role in direct hydrazine fuel cells and presents a promising alternative to the kinetics-sluggish oxygen evolution reaction in water reduction. Engineering catalysts with high-density multifold nanotwin structures has emerged as a compelling strategy to enhance catalytic activity. However, the exploration of multifold nanotwins for HzOR applications remains absent. Herein, we report the successful synthesis of a porous Ni-Zn-Cu catalyst featuring high-density twofold and fivefold nanotwins. The Ni-Zn-Cu catalyst supported on Ni foam (Ni-Zn-Cu/Ni foam) exhibits exceptionally high catalytic activity and stability toward the HzOR, achieving a current density of 204.3 mA cm −2 at 0.0 V vs. RHE and retaining up to 89.1 % after 20 h of continuous electrolysis. Online mass spectrometer (MS) analysis indicates that the Ni-Zn-Cu coating facilitates N N bond cleavage of N 2 H 4 . This study offers valuable insights into the development of multifold nanotwin catalysts for advancing HzOR applications.
研究领域:
材料科学
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催化化学
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能源科学
✓ 已验证
DOI
高影响因子
ACS Applied Energy Materials
·
2024
·
IF 5.4
Xia Wei,Tianyao Wang,Hongbin Dai,Song Li
The hydrazine oxidation reaction (HzOR) is critical for direct hydrazine fuel cells and presents a promising alternative to the kinetics-sluggish oxygen evolution reaction in water splitting. Engineering catalysts with high-density nanotwin structures has emerged as a compelling strategy to enhance catalytic activity. However, such catalysts have to be explored for HzOR applications. This work reports the successful synthesis of a porous Ni–Zn catalyst featuring high-density coherent nanotwins (NT-Ni-Zn). NT-Ni-Zn supported on Ni foam exhibited exceptionally high catalytic activity and stability toward the HzOR, achieving a current density of 212.4 mA·cm–2 at 0.04 V vs reversible hydrogen electrode and retaining up to 93.9% after 15 h of continuous electrolysis. In addition, hydrazine-assisted water electrolysis using NT-Ni-Zn/Ni foam as both the cathode and anode require only a cell voltage of 70 mV to reach 10 mA cm–2. The exceptional HzOR activity of the Ni–Zn catalyst is attributed to the presence of the nanotwin structure, which promotes a favorable d-band center position and facilitates strong hydrazine binding on the twinned surface. This study provides valuable insights into the development of nanotwin catalysts for HzOR advancement.
研究领域:
材料科学
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电化学
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能源转换与存储
✓ 已验证
产品关联
DOI
高影响因子
Journal of Materials Chemistry A
·
2018
·Vol. 6
·期 39
·19201-19209
·
IF 9.931
Guoqiang Liu,Zhongti Sun,Xian Zhang,Haojie Wang,Guozhong Wang,Xiaojun Wu,Haimin Zhang,Huijun Zhao
Electrocatalytic water splitting has been widely accepted as an environmentally friendly approach to generate clean H2. However, the sluggish oxidation half reaction, namely, the oxygen evolution reaction (OER), usually requires a high overpotential, which is the obstacle to high-efficiency overall water splitting to generate H2. Herein, we report the preparation of ultrathin nanosheet array Ni3S2 with a 9–14 nm nanosheet thickness grown directly on a commercial Ni foam substrate (Ni3S2/NF) by in situ vapor-phase hydrothermal (VPH) transformation of the nanosheet array structure Ni(OH)2/NF precursor. As a multifunctional electrocatalyst, the as-fabricated Ni3S2/NF-2 (VPH time of 2 h) displays excellent electrocatalytic activities toward the hydrazine oxidation reaction (HzOR) with a potential of 0.415 V (vs. RHE) to deliver a current density of 100 mA cm−2, an OER with an overpotential of 425 mV obtaining the same current density, and a hydrogen evolution reaction (HER) with an onset potential of −0.05 V (vs. RHE) in 1.0 M KOH media. A two-electrode system is therefore constructed using Ni3S2/NF-2 as both the anode and cathode, capable of achieving 100 mA cm−2 at 0.867 V in 1.0 M KOH with 0.2 M hydrazine. Density functional theory (DFT) calculations reveal that the adsorption of N2H4 molecules on the Ni3S2 (110) is more thermodynamically favourable than H2O, thus contributing to the high HzOR activity.
研究领域:
材料科学
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能源化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Wenxin Wang,Jiangjiang Zhang,Jinsheng Rong,Lanli Chen,Shiqiang Cui
Reducing the size of catalysts and tuning their electronic structure and interfacial properties are key to enhancing catalytic performance. Herein, a series of quantum-sized Co-based nanodot composites, including Co 3 O 4 /C, CoS 2 /C, CoN/C, and CoP/C, were synthesized using chemical vapor deposition (CVD) methods. By means of experimental measurement and theoretical calculation, CoP/C exhibited more robust electrochemical response than other Co-based compounds in electrochemical oxidation of N 2 H 4 (HzOR) and hydrogen evolution reaction (HER). The catalytic activities of CoP/C can be further enhanced by introducing Co vacancies on the surface of CoP/C (labeled as Co 1−x P/C). The results demonstrated that Co 1−x P/C not only exhibited notable electrochemical responses at an ultra-low N 2 H 4 concentration of 0.67 μM, showcasing its potential for ultra-sensitive N 2 H 4 detection but also realized HzOR instead of the oxygen evolution reaction (OER) half-reaction, thereby lowering the overpotential to 2.0 mV at 10.0 mA cm −2 . Finally, a Zn-hydrazine (Zn-Hz) battery was fabricated as a promising energy conversion device, showing the exceptional practical value of Co 1−x P/C.
研究领域:
材料科学
·
电化学
·
能源转换
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2021
·
IF 4.464
Siqi Song,Yang Li,Yanfeng Shi,Yuanhong Xu,Yusheng Niu
Direct hydrazine fuel cells (DHFCs) fuel has drawn significant attention due to its characteristics of high energy density. Substantial effort is still needed to explore sustainable and efficient catalysts for hydrazine oxidation reaction (HzOR). Herein, inspired by reducing solvents that can protect the precursors of nanomaterials from oxidation, oxygen-doped MoS 2 nanoflowers with sulfur vacancies (O-rich MoS 2 ) were prepared via a simple synthesis method using the readily available ethanol/water as the solvent and applied as electrocatalyst for HzOR. It is found that the ratio of ethanol to water has a significant influence on the morphology of MoS 2 and the catalytic performance of hydrazine oxidation. Moreover, the concept of O-doping is proposed by introducing oxygen atoms to mostly replace bulk S atoms in the oxidation process of nanomaterials. The sulfur vacancy and doping were regarded as the main active site for the HzOR. Accordingly, the onset potential of the prepared electrocatalyst is 0.5 V vs. RHE in a 1 M KOH/0.1 M hydrazine electrolyte. This doping method can provide new ideas for improving the construction of hydrazine oxidation catalysts in the future.
研究领域:
材料科学
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电化学
·
能源催化
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2022
·
IF 4.889
Weijie Zhu,Appala Gandi Naidu,Qiongfei Wu,Hao Yan,Mengting Zhao,Zhoucheng Wang,Hanfeng Liang
The application of proton exchange membrane water electrolyzer (PEMWE) technology has long been limited by the excessive energy consumption and poor catalyst durability because of the harsh corrosive and oxidative conditions that are related to the anodic oxygen evolution reaction (OER) in acidic electrolytes. Herein, we circumvent this challenge by adopting alternative hydrazine oxidation reaction (HzOR) as the anodic half-reaction, integrated with the cathodic hydrogen evolution reaction (HER) for sustainable hydrogen production. To this end, we further developed a PtCo alloy nanosheets electrocatalyst that can efficiently catalyze both the HzOR and HER with ultralow potentials. Specifically, the overall hydrazine splitting driven by the PtCo alloy requires only 0.28 V at 10 mA cm −2 along with outstanding stability of more than 3000 h. We further proposed a PEM hydrazine electrolyzer (PEMHE) design to promote the practical application. The device can not only produce hydrogen with a high yield rate of 1.87 mmol h −1 cm −2 at a practical current density of 100 mA cm −2 with a long durability of 60 h, but also effectively decontaminate hydrazine sewage with the hydrazine removal efficiency up to 100%. Our work provides a new solution to simultaneous mass hydrogen fuel production and hydrazine hazard removal from acidic waste water at minimized energy consumption.
研究领域:
能源科学
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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
Journal of Materials Chemistry A
·
2023
·Vol. 11
·期 19
·10222-10227
·
IF 11.9
Ziqiang Wang,Guanghui Yang,Pengjun Tian,Kai Deng,Hongjie Yu,You Xu,Xiaonian Li,Hongjing Wang,Liang Wang
Water electrolysis for hydrogen production consumes abundant electronic energy owing to the sluggish oxygen evolution reaction (OER), so the integration of the hydrogen evolution reaction (HER) with thermodynamically more favorable oxidation reactions is a promising strategy for energy-efficient hydrogen production. Herein, we propose the epitaxial confinement of rhodium nanoparticles (NPs) to palladium metallene (Rh/Pd metallene) for hydrogen production assisted by the hydrazine oxidation reaction (HzOR). The two-dimensional structure of Rh/Pd metallene provides sufficient active sites as well as a rapid charge transfer rate. The interface of Pd metallene with Rh NPs ensembles to modulate the electronic state, thus optimizing the adsorption energy of reaction intermediates. The Rh/Pd metallene exhibits splendid HER and HzOR activities, with overpotentials of 59 and 7 mV at 10 mA cm−2, respectively. In the two-electrode construction of a hydrazine oxidation-assisted water splitting system, the Rh/Pd metallene only needs a low overpotential of 0.19 V to produce hydrogen at a current density of 100 mA cm−2. This research offers a viable approach for designing nanosheet/nanoparticle heterojunction as an attractive modular platform for energy-saving hydrogen production.
研究领域:
材料科学
·
能源化学
✓ 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）