JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Xiaofeng Ke,Feng Zhou,Yihuang Chen,Mei Zhao,Yun Yang,Huile Jin,Youqing Dong,Chao Zou,Xi'an Chen,Lijie Zhang,Shun Wang
Sluggish kinetics of hydrogen oxidation reaction (HOR) in alkaline solution has restricted the rapid development of hydrogen economy. Constructing catalyst with metal-oxide heterostructures can enhance HOR performance; however, little studies concentrate on charge transfer between them, and the corresponding effects on reactions remain unclear. Herein, we report charge-transfer-adjustable CeO 2 /Rh interfaces uniformly dispersed on multiwalled carbon nanotube (CNT), which exhibit excellent alkaline HOR performance. Results confirm that the charge transfer from Rh to CeO 2 could be conveniently tuned via thermal treatment. Consequently, the adsorption free energies of H* in Rh sites and OH* adsorption strength in CeO 2 could be adjusted, as corroborated by density functional theory study. The optimized CeO 2 /Rh interfaces exhibit an exchange current density and a mass-specific kinetic current of 0.53 mA cm PGM −2 and 830 A g PGM −1 at an overpotential of 50 mV, respectively, which surpasses most of the advanced noble-metal-based electrocatalysts. This work provides a new insight of harnessing charge transfer of heterostructure to enhance catalytic activities.
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Catalysis
·
2023
·
IF 12.9
Xu Yu,Han Tian,Zhengqian Fu,Fenglai Pei,Lingxin Peng,Ge Meng,Fantao Kong,Yafeng Chen,Chang Chen,Ziwei Chang,Xiangzhi Cui,Jianlin Shi
The hydrogen spillover effect on metal-supported electrocatalysts is of great significance in hydrogen-involved reactions, especially in a hydrogen oxidation reaction (HOR). Herein, a facile thermal reduction method has been adopted to synthesize W18O49 (WO2.72) nanospheres decorated with single nickel atoms, and the obtained Ni-WO2.72-T (1.20 wt % Ni) was used as a probe catalyst for investigating the hydrogen spillover effect, which exhibits enhanced HOR performance, stability, and resistance to CO poisoning in acidic electrolytes. Based on in situ Raman spectroscopy and the density functional theory (DFT) calculation, a synergistic effect between Ni single-atom active sites and the hydrogen spillover effect is proposed to contribute to the HOR performance on Ni-WO2.72-T. Briefly, the introduction of single Ni atoms induces electron redistribution on Ni-WO2.72-T, making Ni atoms positively charged for H2 adsorption and activation, and on the other hand, the reversible phase transformation between WO2.72 and HxWO2.72 facilitates H* transfer from Ni to WO2.72, i.e., hydrogen spillover, resulting in elevating the HOR catalytic activity. Both experimentation and theoretical calculations demonstrate that the reversible phase transformation of the WO2.72 substrate strengthens the hydrogen spillover effect and thus elevates the HOR catalytic performance, which is believed to be helpful in designing highly active catalysts for hydrogen-involving reactions.
研究领域:
电化学
·
催化材料
·
理论计算
✓ 已验证
产品关联
DOI
高影响因子
ACS Catalysis
·
2022
·
IF 13.7
Chang Sun,Pengcheng Zhao,Yongqing Yang,Zhuo Li,Wenchao Sheng
The application of anion exchange membrane fuel cells is hampered by the development of highly efficient and earth-abundant anode hydrogen oxidation reaction (HOR) catalysts. Here, a series of nickel catalysts (denoted as Ni-X) with different lattice oxygen (LO) contents were synthesized by H2 reduction of nickel hydroxide at temperatures (X) ranging from 300 to 500 °C. The Ni-400 (LO/Ni = 0.41, NiO0.41) catalyst with an optimum LO content showed excellent HOR activity and stability, comparable to current Ni-based electrocatalysts. An X-ray photoemission spectroscopic study, combined with density functional theory calculations, suggested that introducing LO into Ni modified the metal d-band electronic structure and in turn the hydrogen binding energy, which played a major role in determining the HOR 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 Materials Chemistry A
·
2024
·
IF 10.7
Xu Yu,Han Tian,Ziyi Yu,Fantao Kong,Chang Chen,Ziwei Chang,Jian Huang,Xiangzhi Cui,Jianlin Shi
Hydrogen spillover effect-based active catalyst design is an effective strategy to enhance the hydrogen oxidation reaction (HOR) performance, which, unfortunately, still suffers from the high hydrogen spillover energy barrier. Here, a strategy alloying Ir with Ru is proposed to modulate the electronic structure of Ir to accelerate the H* transfer by a novel Ir–Ru–WO2.72 bridge, thus significantly reducing the hydrogen spillover energy barrier from Ir to WO2.72. The IrRu nanoclusters were deposited on a three-dimensional ordered macroporous WO2.72–C framework, and thus the constructed IrRu–WO2.72–C (1.16 wt% Ir and 1.09 wt% Ru) catalyst exhibits excellent HOR and CO-tolerance performance, rather high cell power density, and especially, 4 times higher mass activity than that of Pt/C. The modulation of Ru largely decreases the work function difference between the IrRu clusters and substrate, resulting in a reduced hydrogen spillover barrier via the Ir–Ru–WO2.72 bridge, weakened CO adsorption and fast removal of the adsorbed CO.
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Jiwen Lin,Zhongyao Zhang,Jiaye Qiu,Yujie Wu,Jun Yu,Yongliang Li,Xiangzhong Ren,Lei Zhang,Zhongxin Song
Pt-based catalysts are widely used in hydrogen oxidation reaction (HOR) for the anode of proton exchange membrane fuel cells (PEMFCs). However, high Pt loading and CO poisoning increase the overall cost and stringent requirements for fuel purity. Here, decreasing Pt usage while achieving high anode performance by anchoring Ni single atoms under or adjacent to Pt nanoclusters is studied. The electron interaction between oxophilic Ni single atoms and Pt nanoclusters is beneficial for optimizing the electrocatalytic HOR. The Pt-Ni SA /CNT-2.6 (CNT-carbon nanotube) catalyst with 2.6 wt% low Pt loading shows superior catalytic activity for the HOR, long-time stability, and good CO-tolerant performance in the liquid half-cell and fuel cell of membrane electrode assembly (MEA). Theoretical calculations reveal that the synergy between single atoms and nanoclusters optimizes the d band of Pt and decreases the activation barrier for HOR and CO stripping, thereby enhancing HOR activity and high CO tolerance in PEMFC anodes with a low Pt loading. This work provides a novel design of electron interactions between single atoms and Pt nanoclusters, showing a significant advantage in promoting low-Pt PEMFCs with high power and CO tolerance.
研究领域:
材料科学
·
电化学
·
燃料电池
✓ 已验证
产品关联
DOI
高影响因子
Science Bulletin
·
2022
·
IF 20.577
Juntao Zhang,Guomian Ren,Deyu Li,Qingyu Kong,Zhiwei Hu,Yong Xu,Suling Wang,Lu Wang,Maofeng Cao,Xiaoqing Huang
Ru has recently been regarded as a promising catalyst for hydrogen oxidation reaction (HOR) and hydrogen evolution reaction (HER) due to its similar binding energy towards *H but lower price compared to Pt. Nevertheless, the quest of high-efficiency Ru-based catalysts for HOR and HER is driven by the current disadvantages including low activity and unsatisfactory stability. Herein, we have fabricated and engineered two-dimensional (2D) Ru-based snow-like nanosheets with Ru/RuO 2 interface (Ru/RuO 2 SNSs) via a post-annealing treatment. Detailed characterizations and theoretical calculations indicate that the interfacial synergy, which is dependent on the temperature for annealing, can alter the hydrogen binding energy (HBE) and hydroxide binding energy (OHBE), as a result of the enhanced HOR and HER performance. Impressively, the optimal Ru/RuO 2 SNSs display a mass activity of 9.13 A mg Ru –1 at an overpotential of 50 mV in 0.1 mol L –1 KOH for HOR, which is 65, 304, and 21 times higher than those of Ru SNSs (0.14 A mg Ru –1 ), RuO 2 SNSs (0.03 A mg Ru –1 ), and commercial Pt/C (0.43 A mg Ru –1 ), respectively. Moreover, Ru/RuO 2 SNSs display improved HER activity with a low overpotential of 20.2 mV for achieving 10 mA cm −2 in 1 mol L –1 KOH. This work not only provides an efficient catalyst for HOR and HER, but also promotes fundamental research on the fabrication and modification of catalysts in heterogeneous catalysis .
研究领域:
材料科学
·
电催化
·
能源化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2023
·
IF 7.2
Liming Zeng,Tianxiang Yuan,Yongyang Zhu,Daifeng Wu,Qing Zhou,Renheng Tang
For hydrogen oxidation reaction (HOR), the kinetics in alkaline media is much sluggish than that in acidic media, and its catalyst mainly relies on noble metal-based materials, so it is of great significance to develop non-noble metal-based efficient HOR catalysts. In this work, based on the strong coordination interaction between transition metal cation and ligand molecule with lone pair electrons , a novel type of nickel-based aerogel-like material (Ni@NiO/C-400) is elaborately constructed. The material is composed of a spongy three-dimensional skeleton and a coated ultrathin layer，while the former is formed by the interconnection of metallic nickel nanorods and the latter contains nickel oxide species and embedded graphitic carbon island. The Ni@NiO/C-400 present certain exchange current density , kinetic current density and mass activity, implying obvious HOR activity. Based on the physicochemical characterization results, the Ni/NiO interface layer is formed on the catalyst surface and is supposed to provide moderate binding energy for H∗ and OH∗ and proposed to be a crucial origin of activity. Due to the accessible adsorption of intermediate species, exposure of active sites and protection for metallic nickel from over-oxidation, along with the favorable electronic conductivity enabled by the embedded graphitic carbon , the unique uneven thin layer on the catalyst surface also plays an important role in catalyzing HOR. Additionally, the three-dimensionally porous nickel framework endows abundant channels for electron transport and mass transfer during alkaline HOR process. The material-architecting strategy proposed in this work paves a new avenue for the rational design of non-noble metal catalysts .
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Yuanjun Liu,Yiru Wu,Kunpeng Yang,Jun Yu,Junhao Zhang,Guoxing Zhu
Reasonable design of efficient and environmentally friendly alkaline hydrogen oxidation (HOR) electrocatalysts is urgently required for the development of alkaline hydrogen-oxygen fuel cells. In this work, carbon dots (CDs) were coupled with ruthenium (Ru) to form a hybrid Ru/CDs electrocatalyst. The combination of CDs with Ru nanoparticles can effectively inhibit the aggregation of Ru nanoparticles. Moreover, the electronic structure of Ru is modified due to the interaction between Ru and CDs. The optimized Ru/CDs catalyst exhibited excellent alkaline HOR activity with an exchange current density of 1.56 mA cm −2 that is significantly better than commercial Pt/C catalysts. These findings considerably broaden the potential applications of CDs and provide additional options for the development of high-performance HOR electrocatalysts.
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
Advanced Energy Materials
·
2025
·
IF 26
Guimei Liu,Yushen Liu,Xiaoyi Qiu,Bingxing Zhang,Juhee Jang,Yingdan Cui,Fei Xiao,Qinglan Zhao,Wenjun Wang,Yoonseob KIM,Wei Xing,Minhua Shao
The slow reaction kinetics of hydrogen oxidation reaction (HOR) on existing catalysts in alkaline hinders the commercialization of anion exchange membrane fuel cells (AEMFCs). In this work, a Cu-incorporated NiW alloy (Cu i -NiW) without any platinum group metal (PGM) is designed and evaluated in both liquid cells and AEMFCs. This catalyst enabled the achievement of an electrochemical surface area-normalized exchange current density of 70 µA cm −2 and robust stability, outperforming most PGM-free catalysts. Furthermore, the incorporation of Cu into other systems such as NiMo and NiV using the same method also showcased excellent HOR activity and durability. The fuel cells assembled with Cu i -NiW as the anode and Pt/C or Fe-N-C as the cathode delivered peak power densities of 480 and 340 mW cm −2 , respectively. Experimental and theoretical studies reveal that the incorporated Cu is chemically inert but enhances the overall oxidation resistance of the catalysts. Moreover, it weakens hydrogen adsorption and promotes the adsorption of hydroxide ions, thereby enhancing the HOR activity significantly. These results may open a door for rational design of high-performance and durable PGM-free HOR catalysts.
研究领域:
电化学
·
催化材料
·
能源科学
✓ 已验证
DOI
高影响因子
Journal of the American Chemical Society
·
2022
·
IF 16.383
Xiaodong Yang,Bo Ouyang,Peiqi Shen,Yiqiang Sun,Yisong Yang,Yanan Gao,Erjun Kan,Cuncheng Li,Kun Xu,Yi Xie
Developing efficient hydrogen oxidation reaction (HOR) electrocatalysts in alkaline media is of great significance for anion exchange membrane fuel cells. Herein, we report the synthesis of hollow colloidosomes composed of Ru nanocrystals based on a novel gas/liquid interface self-assembly strategy. Structural characterizations reveal that much defects are present in the building block (Ru nanocrystals) of Ru colloidosomes. Theoretical calculations suggest that the defects in the Ru structure can optimize the adsorption binding energy of reaction intermediates for the HOR. Benefiting from the assembled colloidosome and optimized electronic structure, the Ru colloidosomes exhibit remarkable HOR catalytic performance in alkaline media with a mass activity higher than that of benchmark Pt/C. Our work may shed new light on the rational design of advanced electrocatalysts with an assembled structure for energy-related applications.
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
JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
·
IF 6.2
Yuanjun Liu,Longkun Zuo,Yuyu Liu,Yiru Wu,Xingmei Guo,Junhao Zhang,Fu Cao,Xiangjun Zheng,Guoxing Zhu
Hydrogen oxidation reaction (HOR) with alkaline solution is an important process for anion exchange membrane hydrogen-oxygen fuel cells, while it presents slow kinetics because it contains the coupling of adsorbed hydrogen (H ad ) and hydroxyl (OH ad ) species. Herein, PtRu alloy network-like structure with small size was prepared by a solution phase reduction route, which acts as an electrocatalyst for HOR. The presence of Ru changed the d -band center of Pt and so optimized the hydrogen bonding energy on Pt sites. At the same time, Ru species provides functional surface for the adsorption of OH species. The ultrathin size of the alloy units provides richness of exposed active sites for HOR. Benefited from the above factors, the obtained PtRu alloy with Pt:Ru ratio of 1:1 shows the optimized catalytic activity, providing an exchange current density of 1.93 mA cm −2 , which is 2.7-fold and 1.5-fold of those for commercial Pt/C and pristine Pt catalyst, respectively. This work provides a new advanced electrocatalyst for alkaline HOR.
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 Energy Chemistry
·
2025
·
IF 14.9
Chenggong Niu,Yi Liu,Shuqing Zhou,Heyang Liu,Linyu Chen,Jingya Guo,Tayirjan Taylor Isimjan,Xiulin Yang
Triggering structural asymmetry can induce charge redistribution and modify electronic structures, which is of great significance for the design of high-performance hydrogen oxidation reaction (HOR) electrocatalysts. Herein, we propose a dual anion-induced strategy to create an innovative RuS 2 -RuO 2 heterostructure featuring abundant S-Ru-O interfaces (RuS 2 -RuO 2 @C). This RuS 2 -RuO 2 @C demonstrates an impressive mass activity of 2.61 mA μ g R u - 1 and an exchange current density of 2.96 mA cm −2 , surpassing Pt/C and other comparative samples by over 20 times. Durability assessments confirm the superior stability of RuS 2 -RuO 2 @C, with only minimal performance loss during operation. Density functional theory (DFT) calculations indicate that the asymmetric S-Ru-O configuration optimizes the interfacial electronic structure and shifts the d -band center closer to the Fermi level, effectively reducing the energy barrier of the rate-determining step (RDS) in the alkaline HOR process. Moreover, in situ attenuated total reflection surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS) characteristics disclose the formation of a substantial hydrogen bond network at the S-Ru-O interface, which aids in the desorption of H 2 O ad and facilitates the vital Volmer step in the HOR pathway.
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
危险品化学品经营许可证（带存储）