ACS Nano
·
2023
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IF 17.1
Liyuan Wang,Shuang Meng,Chongyang Tang,Changhong Zhan,Shize Geng,Kezhu Jiang,Xiaoqing Huang,Lingzheng Bu
The development of high-performance platinum (Pt)-based electrocatalysts for the hydrogen oxidation reaction (HOR) is highly desirable for hydrogen fuel cells, but it is limited by the sluggish kinetics and severe carbon monoxide (CO) poisoning in alkaline medium. Herein, we explore a class of facet-selected Pt–nickel–indium fishbone-like nanowires (PtNiIn FNWs) featuring high-index facets (HIFs) of Pt3In skin as efficient alkaline HOR catalysts. Impressively, the optimized Pt66Ni6In28 FNWs show the highest mass and specific activities of 4.02 A mgPt–1 and 6.56 mA cm–2, 2.0/2.1 and 13.9/15.6 times larger than those of commercial PtRu/C and commercial Pt/C, respectively, along with a competitive CO-tolerance ability. Specifically, they exhibit only 6.0% current density decay after 10000 s of operation and 25.7% activity loss after 2000 s in the presence of 1000 ppm of CO. Moreover, an isotope experiment and density functional theory (DFT) calculations further prove that the unique structure and synergy among Pt, Ni, and In endow these Pt66Ni6In28 FNWs with an optimized hydrogen binding energy (HBE) and an advantageous hydroxide binding energy (OHBE), giving them excellent alkaline HOR properties. The combined construction of surface-skin and HIFs in PtNiIn FNWs will offer an available method to realize the potential applications of advanced non-PtRu-based catalysts in fuel cells and beyond.
研究领域:
材料科学
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电化学
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催化
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纳米技术
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DOI
PubMed
高影响因子
Energy Technology
·
2025
·Vol. 13
·期 9
·2402044
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IF 3.6
Dan Lu,Guang Zhu,Wei Liu,Kaixin Wang,Qixuan Wang,Chenxi Xu
The Pt/C catalysts applied in proton exchange membrane fuel cell (PEMFC) suffer CO poisoning in the anode, which notably deteriorates the device performance. The metal–support interaction that decreases the CO oxidation stripping potential is a suitable way to prevent CO anchoring the active sites that can reduce or even avoid the poisoning. Herein, the Pt is supported by amorphous NbO x ( x = 1.0–2.5) and CNT to form Pt@NbO x + CNT catalyst, which not only displays the lower initial and peak CO oxidation stripping potential but also exhibits the striking anti-CO poisoning and hydrogen oxidation reaction properties. The initial and peak potential for oxidation stripping of Pt@NbO x + CNT catalyst are 0.162 and 0.332 V, respectively. Moreover, the PEMFC based on Pt@NbO x + CNT catalyst in 100 ppm CO/H 2 exhibits a peak power density of 1.98 W cm −2 , only 17% reduction compared to that in pure hydrogen and the catalyst remains 10 h stability at 0.4 V.
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高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-11
·
IF 14.7
Huang Zhongliang,Hu Shengnan,Sun Mingzi,Xu Yong,Liu Shangheng,Ren Renjie,Zhuang Lin,Chan Ting-Shan,Hu Zhiwei,Ding Tianyi,Zhou Jing,Liu Liangbin,Wang Mingmin,Huang Yu-Cheng,Tian Na,Bu Lingzheng,Huang Bolong,Huang Xiaoqing
Bimetallic PtRu are promising electrocatalysts for hydrogen oxidation reaction in anion exchange membrane fuel cell, where the activity and stability are still unsatisfying. Here, PtRu nanowires were implanted with a series of oxophilic metal atoms (named as i-M-PR), significantly enhancing alkaline hydrogen oxidation reaction (HOR) activity and stability. With the dual doping of In and Zn atoms, the i-ZnIn-PR/C shows mass activity of 10.2 A mg Pt+Ru −1 at 50 mV, largely surpassing that of commercial Pt/C (0.27 A mg Pt −1 ) and PtRu/C (1.24 A mg Pt+Ru −1 ). More importantly, the peak power density and specific power density are as high as 1.84 W cm −2 and 18.4 W mg Pt+Ru −1 with a low loading (0.1 mg cm −2 ) anion exchange membrane fuel cell. Advanced experimental characterizations and theoretical calculations collectively suggest that dual doping with In and Zn atoms optimizes the binding strengths of intermediates and promotes CO oxidation, enhancing the HOR performances. This work deepens the understanding of developing novel alloy catalysts, which will attract immediate interest in materials, chemistry, energy and beyond.
研究领域:
材料科学
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化学
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能源
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DOI
PubMed
高影响因子
ADVANCED MATERIALS
·
2025
·
IF 26.8
Yanfu Tong,Xuejin Li,Xiaoning Wang,Lianming Zhao,Weiyue Luo,Zhenyu Huang,Pengyun Liu,Zifeng Yan,Yuan Pan,Wei Xing
Breaking scaling relations and overcoming kinetic limitations in multistep hydrogen electrocatalysis remains a fundamental challenge. In this work, we designed and synthesized a high-entropy alloy catalyst comprising Ir, Ru, Mo, W, and Cu supported on nitrogen-doped carbon spheres. This unique structure creates active sites with a quasi-continuous distribution of binding energies for H* and OH* intermediates. Density functional theory (DFT) calculations confirm that the random spatial arrangement of sites enables low-energy-barrier spillover pathways for H* and OH* (χ H* max = 0.27 eV; χ OH* max = 0.61 eV), while continuous d-orbital coupling facilitates efficient electron transfer. This design enables each elementary step of hydrogen oxidation and evolution reactions (HOR/HER) to be directed to a site with favorable energetics. As a result, it exhibits exceptional bifunctional performance with a HOR mass activity of 8.83 A mg −1 and an HER overpotential of only 11 mV at 10 mA cm −2 , significantly outperforming commercial Pt/C com and previously reported catalysts. Operando spectroscopy and DFT analyses reveal that the gradient energy landscape promotes dynamic intermediate spillover, preventing site blocking and enhancing reaction kinetics. This work establishes a universal design strategy develop high-performance electrocatalysts that transcend conventional Sabatier principle limitations.
研究领域:
电催化
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材料科学
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能量转换
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计算化学
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纳米材料
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DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2024
·
IF 20.2
Yi Liu,Lianrui Cheng,Shuqing Zhou,Chenggong Niu,Tayirjan Taylor Isimjan,Xiulin Yang
Exploiting a cost-effective electrocatalyst for hydrogen oxidation reaction (HOR) with high-performance and CO poisoning resistance is essential for the widespread application of alkaline anion exchange membrane fuel cells (AEMFCs). Herein, we craft a unique Ru-RuP 2 heterostructure within hollow mesoporous carbon sphere (Ru-RuP 2 @C) using phosphide-controlled phase-transition approach. Benefiting from the interfacial electron transfer from RuP 2 to Ru, the Ru-RuP 2 @C electrocatalyst exhibits impressive HOR performance with a mass activity of 2.87 mA μ g Ru − 1 . Notably, Ru-RuP 2 @C demonstrates strong tolerance to 1000 ppm CO, a capability lacking in PtRu/C and Pt/C. When serves as an anode catalyst for AEMFC, it achieves a peak power density of 521 mW cm −2 , comparable to Pt/C. Experimental and theoretical analyses reveal that the built-in electric field, resulting from work function differences, creates an asymmetric charge distribution that modulates the d -band center of Ru-RuP 2 @C. This optimizes the adsorption strength of hydrogen and hydroxide intermediates, thereby accelerating HOR catalytic kinetics.
研究领域:
电化学
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材料科学
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能源材料
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催化
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DOI
高影响因子
Advanced Energy Materials
·
2022
·Vol. 13
·期 1
·2202913
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IF 29.698
Dan-Qing Liu,Zhouxin Luo,Bingxing Zhang,Guoqiang Zhao,Wei Guo,Jian Chen,Mingxia Gao,Yongfeng Liu,Hongge Pan,Wenping Sun
The sluggish kinetics of hydrogen oxidation reaction (HOR) is one of the critical challenges for anion exchange membrane fuel cells. Here, we report epitaxial growth of Ir nanoclusters (<2 nm) on a MoS 2 surface (Ir/MoS 2 ) and optimize the alkaline HOR activity via tailoring interfacial charge transfer between Ir clusters and MoS 2 . The electron transfer from MoS 2 to Ir clusters can effectively prevent the oxidation of Ir clusters, which is not the case for carbon-supported Ir nanoclusters (Ir/C) synthesized using the same method. Moreover, the HOR performance of the Ir/MoS 2 can be further optimized by tuning the hydrogen binding energy (HBE) via a precise annealing treatment. A substantial exchange current density of 1.28 mA cm ECSA −2 is achieved in the alkaline medium, which is ∼10 times over that of Ir/C. The HOR mass-specific activity of Ir/MoS 2 heterostructure is as high as 182 mA mg Ir −1 . The experimental results and density functional theory calculations reveal that the significant improved HOR activity is attributed to the decreased HBE, which highlights epitaxial growth is an effective way for boosting catalytic activity of heterostructured catalysts.
研究领域:
材料科学
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电化学
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催化
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燃料电池技术
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产品关联
DOI
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-12
·
IF 14.7
Jiang Xiaoyi,Ke Le,Zhao Kai,Yan Xiaoyu,Wang Hongbo,Cao Xiaojuan,Liu Yuchen,Li Lingjiao,Sun Yifei,Wang Zhiping,Dang Dai,Yan Ning
Electrochemical carbon dioxide reduction reaction using sustainable energy is a promising approach of synthesizing chemicals and fuels, yet is highly energy intensive. The oxygen evolution reaction is particularly problematic, which is kinetically sluggish and causes anodic carbon loss. In this context, we couple CO 2 electrolysis with hydrogen oxidation reaction in a single electrochemical cell. A Ni(OH) 2 /NiOOH mediator is used to fully suppress the anodic carbon loss and hydrogen oxidation catalyst poisoning by migrated reaction products. This cell is highly flexible in producing either gaseous (CO) or soluble (formate) products with high selectivity (up to 95.3%) and stability (>100 h) at voltages below 0.9 V (50 mA cm −2 ). Importantly, thanks to the “transferred” oxygen evolution reaction to a water electrolyzer with thermodynamically and kinetically favored reaction conditions, the total polarization loss and energy consumption of our H 2 -integrated CO 2 reduction reaction, including those for hydrogen generation, are reduced up to 22% and 42%, respectively. This work demonstrates the opportunity of combining CO 2 electrolysis with the hydrogen economy, paving the way to the possible integration of various emerging energy conversion and storage approaches for improved energy/cost effectiveness.
研究领域:
电化学
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能源转换与存储
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可持续能源
✓ 已验证
产品关联
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
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IF 8.1
Pengyu Wei,Yaxin Lv,Changyang Liu,Ziliang Liu,Lilin Yang,Ruixue Tian,Jun Peng,Liuzhen Bian,Shengli An
Perovskite oxide-based materials are promising electrode materials for reversible symmetric solid oxide cells (RSSOCs) as they exhibit good catalytic activity and stability in oxidizing and reducing atmospheres. In this study, A-site deficient (La 0.5 Sr 0.5 ) 0.95 Fe 0.9 Mo 0.1 O 3-δ (95LSFMo) is synthesized as an electrode material for RSSOCs. The A-site defect in La 0.5 Sr 0.5 Fe 0.9 Mo 0.1 O 3-δ increases the surface oxygen vacancy concentration, promoting the transport of oxygen ions and enhancing the catalytic activities of oxygen reduction (ORR) and hydrogen oxidization reaction (HOR). 95LSFMo|LSGM|95LSFMo symmetric cell achieves a maximum power density (MPD) of 1.14 W cm −2 at 850 °C. Furthermore, the adsorption and reduction of H 2 O is also improved. In 50 %H 2 O-H 2 , 95LSFMo cell shows a current density of −1.71 A cm −2 at 850 °C and 1.3 V in electrolysis mode and a peak power density of 0.82 W cm −2 in fuel cell mode. The corresponding hydrogen production rate reaches 714.78 ml cm -2 h −1 . Moreover, the 95LSFMo cell exhibits good reversibility as well as SOEC stability.
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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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Junlin Cai,Xinyan Liao,Pingting Li,Qiuxiang Wang,Hongpu Huang,Zixi Lyu,Jing Lin,Shuifen Xie
Surface defects on electrocatalysts can effectively reduce reaction barriers and facilitate the kinetics of hydrogen evolution and oxidation reactions (HER/HOR). However, precisely engineering such surface structures remains a significant challenge. Herein, penta-twinned (PTw) Rh@Pt x core–shell nanobranches (NBs) with intense surface strains were facilely synthesized using PTw Rh NBs as the seeds for overgrowth of active Pt-shells. Through precisely regulating the supply of Pt precursor solution via a micro-syringe pump, the ultrathin Pt-shells conform to and replicate the twin defects of the PTw Rh seeds. Significantly, the shell thickness can be precisely controlled from 1.0, 2.0, and 3.8 to 5.0 atomic layers. Due to the integration of surface twinned defects, compressive strain and the core–shell ligand effect, these Rh@Pt x NBs exhibit superior hydrogen redox electrocatalytic performance compared to state-of-the-art Pt/C. Among the prepared materials, the Rh@Pt 0.83 NBs with a 3.8 atomic layer Pt-shell showed the highest mass activity (2.36 A mg Pt −1 ) and specific activity (6.55 mA cm −2 ) for HER at –0.07 V and presented the lowest overpotential (44 mV) at 10 mA cm −2 , less than half the overpotential of the commercial Pt/C (98 mV). In terms of HOR, the Rh@Pt 0.83 NBs showed a superior exchange current density (1.97 mA cm −2 ), approximately 7 times higher than that of Pt/C. Our work provides a facile method to synchronously engineer the Pt-shell thickness and surface defects of Rh@Pt core–shell nanocatalysts for the creation of robust and bifunctional hydrogen redox electrocatalysts.
研究领域:
材料科学
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电化学
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纳米技术
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产品关联
DOI
高影响因子
EES Catalysis
·
2025
·
IF 8.1
Jie Yang,Lifang Chen,Xuya Zhu,Wenwen Shi,Mengxue Huang,Chang Liu,Ruimin Ding,Lin Gan,Xi Yin
H2O2 -related electrochemical reactions, including two-electron oxygen reduction reaction (2e-ORR), H2O2 oxidation reaction (HPOR), and H2O2 reduction reaction (HPRR), have received significant attention for the electrosynthesis H2O2 and energy storage. Understanding the complex structure-activity relationships among 2e-ORR/ HPOR/HPRR and their connections is crucial for further developing highly efficient catalysts and working systems. Herein, we unveil these intricacies by employing model Co-N-C catalysts with well-defined active site configuration (Co-N4-pyrrolic and Co-N4- pyridinic ) in a combined experimental and computational approach. We report the higher 2e-ORR/HPOR but lower HPRR activity of CoN4-pyrrolic site than the CoN4-pyridinic site based on their reaction free energy landscapes remodeled considering the chemisorption steps of O2 and H2O2 . The results reveal that the binding free energy of *OOH (ΔG*OOH ) can only be utilized as a reliable descriptor for 2e-ORR/HPOR activity, but not indicative of HPRR activity, regardless of the scaling relationship of the common reaction intermediates ( *OOH or *OH). The HPRR activity of CoN 4 sites strongly depends on the H2O2 adsorption strength and configuration. These findings provide valuable insights into the design of catalysts for H2O2 -related electrochemical energy conversion and storage systems.
研究领域:
电化学
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催化
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材料科学
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能量转换与存储
·
计算化学
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产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Yang Peng,Churong Huang,Meiling Pan,Xin Yue,Shaoming Huang
The development of efficient nonprecious metal catalysts for the alkaline hydrogen oxidation reaction (HOR) catalyst in alkaline anion-exchange membrane fuel cells (AEMFCs) is of great significance. Nickel-based catalysts are considered to be promising HOR catalysts. Here, we report the interfacial engineering of reduced graphene oxide-supported Ni and Ni–Mo bimetallic nitrides (Ni–Ni3Mo3N/rGO), which exhibit excellent catalytic activity of alkaline HOR. The electron transfer from Ni to Ni3Mo3N has been regulated to tune the electronic structure. Due to the interface effect between Ni and Ni3Mo3N, Ni–Ni3Mo3N/rGO exhibits enhanced HOR activity, with a high current density of 2.65 mA cm–2 at an overpotential of 50 mV. Additionally, it demonstrates higher exchange current density (j0, 3.21 mA cm–2) and kinetic current density (jk, 10.35 mA cm–2), indicating fast kinetics and high intrinsic activity of Ni–Ni3Mo3N/rGO. Furthermore, detailed characterization results illustrate that due to the rational adsorption of hydrogen and hydroxyl groups by Ni–Ni3Mo3N/rGO, it possesses significant activity and durability. These research findings are of great importance for the development of more efficient alkaline HOR catalysts to promote the application of alkaline AEMFCs.
研究领域:
催化
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电化学
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材料科学
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能量转换
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燃料电池
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纳米技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Changqing Jin,Fanglin Wu,Haibo Tang,Hongfei Pan,Zhida Chen,Rui Wang,Zihan Meng,Junsheng Li,Haolin Tang
The development of catalysts for hydrogen oxidation reaction (HOR) with enhanced resistance to ammonia poisoning is an important factor in the practical application of hydrogen electrochemical purification devices (HEPDs). This paper reports on the creation of a highly active and anti-ammonia HOR catalyst developed by tuning the charge distribution of the support material through nitrogen-doping of carbon. The nitrogen-doped carbon-supported platinum catalyst (Pt-N 2 /KB, 2.03 wt% Pt) achieves a high mass activity and exchange current density of 2788 mA mg pt -1 and 1020 mA mg pt -1 , respectively, which are 5.4 and 4.7 times higher than that of the comm. 20% Pt/C. The Pt-N 2 /KB catalyst also displays a lower percentage of current decay and enhanced electrochemical stability, indicating superior anti-ammonia toxicity in the tests with HEPD. Density functional theory (DFT) calculations reveal that the hydrogen adsorption free energy (ΔG H* ) on the surface of Pt-N 2 /KB is close to zero and has a lower ammonia adsorption energy, thus accounting for its superior HOR activity and anti- ammonia poisoning ability. Consequently, this work facilitates the implementation of HOR catalysts for anti-ammonia poisoning in the HEPDs, thus accelerating the advancement of ammonia cracking for hydrogen production .
研究领域:
催化
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电化学
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材料科学
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能源工程
·
化工
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DOI
高影响因子
危险品化学品经营许可证（带存储）