Sustainable Materials and Technologies
·
2025
·
IF 9.2
Jingyuan Wei,Yanhui Song,Manyuan Gan,Guodong An,Yongqing Shen,Xiaohui Zhao,Yi Zhang,Peizhi Liu,Bingshe Xu,Junjie Guo
Modifying the catalyst's electronic structure is essential for improving the hydrazine oxidation reaction (HzOR) and alkaline hydrogen evolution reaction (HER), but it is still very difficult. We have developed a new heterostructured electrocatalyst in this work using Ru nanosheets and NiCo layered double hydroxides (LDH). In-situ Raman and theoretical studies show that the heterostructure of Ru/NiCo LDH lowers absorption of hydrogen's Gibbs free energy and the d-band center of Ru/NiCo LDH (from −1.7250 to −1.3341 eV), causing the directed development of interfacial H 2 O (ΔG H* , from 1.65 to 0.23 eV). With an overpotential of 19 and 75 mV to achieve 10 and 100 mA cm −2 for HER, these beneficial characteristics provide the Ru/NiCo LDH with exceptional electrocatalytic capabilities. For HzOR, 10 and 100 mA cm −2 may be produced using just −118 and−112 mV, respectively. The Ru/NiCo LDH electrolyzer also only needs 22 and 223 mV to produce 10 and 100 mA cm −2 , respectively. This work lays the groundwork for developing bifunctional catalysts for the green hydrogen industry.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Xiaofeng Ke,Yun Yang,Feng Zhou,Yihuang Chen,Mei Zhao,Quanlong Xu,Nannan Liu,Chao Zou,Huile Jin,Lijie Zhang,Shun Wang
Binary intermetallic compounds (BIMCs) play a significant role in various catalytic systems. However, the synthesis of BIMCs with different stoichiometric ratios remains challenging, and the corresponding studies toward catalytic performance are scarce. Herein, three kinds of pure-phase rhodium antimonide BIMCs (Rh 2 Sb, RhSb, and RhSb 2 ) were successfully fabricated. Interestingly, Rh 2 Sb BIMC shows the highest activity and long-time stability toward hydrogen oxidation reaction (HOR) in alkaline condition among the prepared samples, reaching a mass normalized kinetic current density of 2.04 A mg PGM -1 (PGM: platinum group metal), which is 7.6 times higher than that of commercial Pt/C com . However, the CO-tolerance performances under 1000 ppm CO/H 2 follows the order: RhSb > Rh 2 Sb > RhSb 2 . Combined with the theoretical calculations, the shift of d-band center of Rh x Sb y BIMCs depends on the Sb content. Accordingly, Rh x Sb y BIMCs with different stoichiometric ratio display varied adsorption energy of *OH, *H and CO, giving rise to the individual HOR activity and resistance to CO poisoning. This work sheds a light on designing efficient BIMCs catalysts for energy conversion.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
ADVANCED MATERIALS
·
2025
·
IF 26.8
Xiaozhong Zheng,Shuxin Zhang,Xinying Zheng,Zhongbin Zhuang,Mingxia Gao,Yongfeng Liu,Hongge Pan,Wenping Sun
Ruthenium (Ru) is a more cost-effective alternative to platinum anode catalysts for alkaline anion-exchange membrane fuel cells (AEMFCs), but suffers from severe competitive adsorption of hydrogen (H ad ) and hydroxyl (OH ad ). To address this concern, a strongly coupled multisite electrocatalyst with highly active cluster-scale ruthenium-tungsten oxide (Ru-WO x ) interface, which could eliminate the competitive adsorption phenomenon and achieve high coverage of OH ad and H ad at Ru and WO x domains, respectively, is designed. The experimental and theoretical results demonstrate that WO x domain functions as a proton sponge to perpetually accommodate the activated hydrogen species that spillover from the adjacent Ru domain, and the resulting WO-H ad species are readily coupled with Ru-OH ad at the heterointerface to finish the hydrogen oxidation reaction with faster kinetics via the thermodynamically favorable Tafel-Volmer mechanism. The AEMFC delivers a high peak power density of 1.36 W cm −2 with a low anode catalyst loading of 0.05 mg Ru cm −2 and outstanding durability (negligible voltage decay over 80-h operation at 500 mA cm −2 ). This work offers completely new insights into understanding the alkaline HOR mechanism and designing advanced anode catalysts for AEMFCs.
研究领域:
材料科学
·
电化学
·
能源科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2020
·
IF 8.758
Yunfei Gao,Hanqing Peng,Yingming Wang,Gongwei Wang,Li Xiao,Juntao Lu,Lin Zhuang
Increasing the antioxidation capability of Ni for the hydrogen oxidation reaction (HOR) is considered important and challenging for alkaline polymer electrolyte fuel cells (APEFCs). Herein, we report a series of Ni-core carbon-shell (Ni@C) catalysts obtained by a vacuum pyrolysis method treated at different temperatures. According to the cyclic voltammetry tests and the HOR tests, Ni@C treated at 500 °C exhibits a much higher Ni core utilization and better catalytic activity toward HOR than the commonly used Ni/C catalyst. Furthermore, X-ray photoelectron spectroscopy characterization shows that a higher percentage of Ni0 appears at the surface of the Ni core of Ni@C than the Ni/C catalyst. The accelerated durability tests, as well as the chronoamperometry tests, suggest that the antioxidation capability of Ni has been obviously improved by the carbon shells. The Raman spectra show that the graphitization degree of the carbon shells might be the key factor affecting the Ni utilization and the HOR catalytic activity of the Ni@C catalysts. The APEFC achieves a peak power density of 160 mW/cm2 using Ni@C-500 °C as the anode, which could also stably discharge for 120 h at 0.7 V.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
PubMed
高影响因子
Advanced Materials Interfaces
·
2022
·Vol. 9
·期 9
·2102193
·
IF 6.389
Pengcheng Wang,Changlai Wang,Yang Yang,Shi Chen,Zhiyu Cheng,Minxue Huang,Huigang Tong,Qianwang Chen
Highly active and low-cost anodic hydrogen oxidation reaction (HOR) catalysts play a significant role in the large-scale application of anion exchange membrane fuel cells (AEMFCs). Herein, a novel anodic HOR electrocatalyst with RuP nanoparticles loaded on N, O codoped porous hollow carbon (RuP/NOC) is prepared. The catalyst exhibits high catalytic activity toward HOR, achieving a kinetic mass activity of 3.25 mA µg –1 PGM at 50 mV, 13 times higher than that of Ru/NOC and even superior to that of Pt/C. Density functional theory (DFT) calculations demonstrate that the transfer of electrons from ruthenium to phosphorus shifts down the d-band center of Ru, weakening the hydroxyl binding energy and decreasing the reaction energy barrier for HOR, thus enhancing the catalytic activity of Ru.
研究领域:
材料科学
·
电化学
·
能源科学
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Wanli Liang,Zixuan Dan,Xiyu Gong,Jinchang Xu,Hongjuan Wang,Yonghai Cao,Hao Yu,Yanshuo Jin,Hao-Fan Wang
The development of hydrogen energy conversion technology offers a solution to the global energy crisis. Hydrogen evolution reaction (HER) and hydrogen oxidation reaction (HOR) are essential for hydrogen production and utilization. Ni-based catalysts are promising alternatives to Pt-group catalysts under alkaline conditions. However, pure Ni exhibits low activity due to H 2 O dissociation/formation limitations in the rate-determining Volmer step. To overcome this bottleneck, we present a heterostructure-induced electron modulation strategy to regulate the spatial proximity of key intermediates within the inner Helmholtz plane, thereby facilitating Volmer step kinetics. Electron depletion at the Ni site shifts its d -band center upward, enhancing the adsorption of *H, *OH, and *H 2 O. This electronic tuning brings *H and *OH closer and elongates the H–OH bonds in *H 2 O, effectively reducing the Volmer barrier, as confirmed by density functional theory (DFT) and in-situ Raman spectroscopy. We demonstrate this concept using a representative heterostructure of nickel and tungsten nitride on nickel foam (Ni/WN@NF), which exhibits excellent electrocatalytic activity, requiring only 20 mV overpotential to achieve 10 mA cm −2 for HER and reaching an exchange current density of 3.99 mA cm −2 for HOR. This work offers a generalizable interfacial approach for modulating local chemical environments in alkaline hydrogen electrocatalysis.
研究领域:
电催化
·
材料科学
·
能源化学
·
表面科学
·
物理化学
✓ 已验证
产品关联
DOI
高影响因子
ELECTROCHIMICA ACTA
·
2024
·
IF 5.5
Jianchao Yue,Pengyu Han,Xinyi Yang,Xiaoqin Ma,Yu Zhang,Liqing Wu,Jianchuan Wang,Wei Luo
Designing non-Pt-based electrocatalysts with high catalytic activity is challenging but extremely desirable for alkaline hydrogen oxidation reaction (HOR). Herein, we successfully design a nitrogen doped carbon shell coated Ru nanoparticles (Ru@NC) catalyst for efficient alkaline HOR. The obtained Ru@NC exhibits an excellent mass activity of 1.279 mA μg PGM -1 , which is 8.1-times, 10.3-times and 3.7-times higher than that of Ru@C, Ru/C and commercial Pt/C. When further employed as the anode catalyst for anion exchange membrane fuel cells (AEMFCs), a peak power density of 1.114 W cm -2 can be achieved for Ru@NC. Density functional theory (DFT) calculations and experimental results indicate that the hydroxyl binding energy (OHBE) is continually enhanced on the catalysts due to the encapsulation of carbon shell and nitrogen doping derived from the upshifted d-band center of Ru sites in catalysts, which is responsible for the enhanced alkaline HOR performance.
研究领域:
材料科学
·
电化学
·
催化科学
✓ 已验证
DOI
高影响因子
Journal of Energy Chemistry
·
2022
·
IF 13.599
Yuting Yang,Yi Huang,Shuqing Zhou,Yi Liu,Luyan Shi,Tayirjan Taylor Isimjan,Xiulin Yang
Surface vacancy defects, as the bridge between theoretical structural study and the design of heterogenous catalysts, have captured much attention. This work develops a metal-organic framework-engaged replacement-pyrolysis approach to obtain highly dispersed Ru nanoparticles immobilized on the vacancy-rich Ni-NiO@C hollow microsphere (Ru/Ni-NiO@C). Fine annealing at 400 °C introduces nickel and oxygen vacancies on Ru/Ni-NiO@C surface, resulting in an improved electrical conductivity and rapid mass-charge transfer efficiency. Ru/Ni-NiO@C with a hollow micro/nanostructure and interconnected meso-porosity favors the maximal exposure of abundant active sites and elevation of hydrogen oxidation reaction (HOR) activity. Experimental results and density functional theory (DFT) calculations reveal that an electronic effect between Ru and Ni-NiO@C, in conjunction with nickel/oxygen vacancies in the NiO species could synergistically optimize hydrogen binding energy (HBE) and hydroxide binding energy (OHBE). The HBE and OHBE optimizations thus created confer Ru/Ni-NiO@C with a mass activity over 7.75 times higher than commercial Pt/C. Our work may provide a constructive route to make a breakthrough in elevating the hydrogen electrocatalytic performance.
研究领域:
材料科学
·
电化学
·
催化
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2024
·Vol. 171
·期 4
·046504
·
IF 3.1
Shufang Shi,Jie Yang,Lifang Chen,Mengxue Huang,Chang Liu,Ruimin Ding,Xi Yin
The hydrogen peroxide oxidation reaction (HPOR) plays a vital role in the emerging H2-H2O2 cycle energy storage system, in which the rational design of HPOR electrocatalyst is essential for achieving high system efficiency. Herein, we establish the HPOR activity trends using structurally well-defined metal phthalocyanines (MPc) as model catalysts via a combined experimental and computational approach. The measured activity sequence follows the order of CoPc > FePc > MnPc > ZnPc > H2Pc > NiPc > CuPc based on their site-normalized exchange current (i0-s). Theoretical calculations indicate that the binding free energy of hydroperoxyl intermediate, HOO*, on MPc (ΔGHOO*) is the activity descriptor for HPOR. A volcano-type activity trend is observed by correlating the logarithm of i0-s (logi0-s) with the ΔGHOO* values and agrees with the theoretical predictions. This HPOR activity trend provides insights into the design of highly active electrocatalysts for HPOR and related energy applications.
研究领域:
电化学
·
催化
·
能量存储
✓ 已验证
产品关联
DOI
高影响因子
Carbon Energy
·
2023
·Vol. 5
·期 7
·e294
·
IF 20.5
Ruisong Li,Daoxiong Wu,Peng Rao,Peilin Deng,Jing Li,Junming Luo,Wei Huang,Qi Chen,Zhenye Kang,Yijun Shen,Xinlong Tian
As a carbon-free energy carrier, hydrogen has become the pivot for future clean energy, while efficient hydrogen production and combustion still require precious metal-based catalysts. Single-atom catalysts (SACs) with high atomic utilization open up a desirable perspective for the scale applications of precious metals, but the general and facile preparation of various precious metal-based SACs remains challenging. Herein, a general movable printing method has been developed to synthesize various precious metal-based SACs, such as Pd, Pt, Rh, Ir, and Ru, and the features of highly dispersed single atoms with nitrogen coordination have been identified by comprehensive characterizations. More importantly, the synthesized Pt- and Ru-based SACs exhibit much higher activities than their corresponding nanoparticle counterparts for hydrogen oxidation reaction and hydrogen evolution reaction (HER). In addition, the Pd-based SAC delivers an excellent activity for photocatalytic hydrogen evolution. Especially for the superior mass activity of Ru-based SACs toward HER, density functional theory calculations confirmed that the adsorption of the hydrogen atom has a significant effect on the spin state and electronic structure of the catalysts.
研究领域:
催化
·
材料科学
·
能源科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
Nature Communications
·
2025
·Vol. 16
·期 1
·1-11
·
IF 15.7
Guo Wei,Zhao Guoqiang,Sun Ziang,Zhang Bingxing,Xin Dongyue,Gao Mingxia,Liu Yongfeng,Zhuang Zhongbin,Liang Hai-Wei,Pan Hongge,Sun Wenping
The hydrogen oxidation reaction (HOR) shows fast kinetics in proton exchange membrane fuel cells (PEMFCs), and has not drawn intense attention. Here, we propose a tandem electrocatalysis concept, decoupling HOR on two independent active sites for accelerated kinetics. As a proof-of-concept application, a Ru-based tandem HOR catalyst is designed, with Ru nanoclusters decorated with Pt single atoms. Experimental and theoretical studies suggest that H 2 dissociation occurs at Ru sites, and then the produced H species migrate to Pt sites followed by the desorption of H + . The strong Ru-H interaction promotes the H 2 dissociation step, while the optimum Pt-H interaction ensures the fast desorption, thereby substantially enhancing the HOR kinetics. In H 2 –O 2 fuel cells, this catalyst enables a peak power density of 1.91 W cm −2 and a high anodic mass activity of 23.12 A mg −1 at 0.9 V iR-free with an ultralow noble metal loading of 5 μg cm −2 . This work advances the development of low-cost anode catalysts for fuel cells and provides more insight into understanding hydrogen electrocatalysis.
研究领域:
能源材料
·
电化学
·
催化
·
纳米技术
·
燃料电池
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Nature Communications
·
2025
·Vol. 16
·期 1
·1-11
·
IF 15.7
Yang Chengdong,Gao Yun,Xing Zhengyu,Shu Xinxin,Zhuang Zechao,Wang Yueqing,Zheng Yijuan,Li Shuang,Cheng Chong,Wang Dingsheng,Zhang Jintao
Uncovering the dynamic structures of water at the electrode-solution interface is crucial for various electrocatalysis processes, where water acts as a proton and electron source. However, precisely controlling the state of water on complex interfaces remains challenging. Inspired by the metalloproteins in natural enzymes, we herein demonstrate that the hydrophilic sulfo-oxygen bridging between Co and Ru sites (Co s -SO-Ru) optimizes interfacial water structure via a favorable hydrogen-bond network, promoting hydrogen oxidation and evolution reactions. Mechanistic studies reveal that the stereoscopic sulfo-oxygen bridges enhance the connectivity of hydrogen-bond network to promote the proton transfer process via repelling cations from the electrode surface. Furthermore, electron donating Co sites reduce the surface oxophilicity of Ru to optimize the adsorption-desorption behaviors of hydroxyl, governing the timely refreshed Ru sites to enhance catalytic performances. Such bioinspired active sites offer a different pathway for the precise design of interfacial water structure to improve electrocatalysis.
研究领域:
电化学
·
催化
·
材料科学
·
仿生工程
·
物理化学
·
纳米技术
✓ 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）