RSC Advances
·
2013
·Vol. 4
·期 2
·794-804
·
IF 2.562
Han Zhu,Ming Zhang,ShengYing Cai,YingTing Cai,Pan Wang,ShiYong Bao,MeiLing Zou,MingLiang Du
A facile approach for the synthesis of uniform, small size and well-dispersed rhodium nanoparticles (RhNPs) on cross-linked polyvinyl alcohol–polyethyleneimine (PVA–PEI) nanofibers has been demonstrated. Various methods were firstly employed to cross-link PVA nanofibers and the cross-linked PVA–PEI nanofibers exhibited good water stability and porous structures after immersing in water for 72 h. Because of the strong chelate effects among the amine groups, hydroxyl groups and Rh3+ ions, uniform RhNPs with an average diameter of about 2.5 ± 0.2 nm can evenly and densely grow throughout the PVA–PEI nanofibers via an in situ reduction. Meanwhile, the better dispersion and smaller size of the RhNPs grown on the nanofibers in comparison with the pre-synthesized RhNPs directly deposited on the nanofibers exhibit the advantages of in situ reduction for size and dispersion control. The successful fabrication of the RhNPs/(PVA–PEI) nanofibers with various densities of well-dispersed RhNPs demonstrates that the strong chelate effects and stabilization of the PVA–PEI nanofibers also play an essential role in the size and dispersion control of RhNPs. The crystal structures, chemical bonding and interactions of the prepared nanofibers were verified using XPS and FTIR spectra and XRD patterns. These novel nanomaterials were fabricated as non-enzymatic electrochemical sensors and exhibit highly electrocatalytic activity towards H2O2.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Lulu Li,Fenyang Tian,Fengyu Wu,Longyu Qiu,Shuo Geng,Menggang Li,Zhaoyu Chen,Weiwei Yang,Yequn Liu,Yongsheng Yu
Ni 4 Mo electrocatalyst stands out as the promising candidate for hydrogen evolution/oxidation reaction (HER/HOR), yet the intensive hydrogen adsorption leads to sluggish kinetics, decreasing hydrogen catalysis efficiency. Herein, the structure of Ni 4 Mo nanoparticles anchored on wafer-biscuit-like N-SrMoO 4 nanorods (Ni 4 Mo/N-SrMoO 4 ) is developed to accelerate reaction kinetics by modulating electronic structure. The designed N-SrMoO 4 support enables strong electronic metal-support interaction with Ni 4 Mo, resulting in a downward shift of d -band center and achieving thermally neutral hydrogen adsorption. Ni 4 Mo/N-SrMoO 4 exhibits HER performance with an ultralow overpotential of 15 mV at 10 mA cm −2 , superior to Pt/C ( η 10 =18 mV). The outstanding exchange current density of 10.2 mA cm −2 for HOR is three times higher than that of Pt/C (3.5 mA cm −2 ). Ni 4 Mo/N-SrMoO 4 is further assembled in anion exchange membrane water electrolyzer (AEMWE), resulting in a current density of 100 mA cm −2 at voltage of 1.71 V and the excellent stability of 300 hours. Theoretical calculations and in-situ spectroscopy indicate that the introduction of Sr in N-SrMoO 4 effectively enhances electronic metal-support interaction, facilitates the enrichment of adsorbed hydroxyl (OH ads ) on active sites and weakens hydrogen adsorption on Ni 4 Mo, thereby accelerating reaction kinetics of hydrogen electrocatalysis.
研究领域:
材料科学
·
电化学
·
催化科学
✓ 已验证
产品关联
DOI
高影响因子
Materials Today Chemistry
·
2023
·
IF 7.3
W. Tang,L. Zhang,H. Huang,Y. Luo,C. Dong,D. Zhou,A. Li,W. Dong,G. Wang,Y. He
The development of efficient catalysts is essential to promote slow hydrogen reaction kinetics in alkaline solutions. Herein, an ultrathin ZIF-derived efficient HOR/HER electrocatalyst , with Co single-atom-anchored RuCo clusters on N-doped graphitized carbon nanosheets (RuCo/SANC NS), is designed and constructed by a step-by-step calcination strategy. In the RuCo/SANC NS, Co atoms dispersed in carbon nanosheets induce the formation of ultrasmall RuCo clusters and stabilize the RuCo clusters. Abundant coordinatively unsaturated Ru sites are formed on the surface of RuCo clusters due to the small size effect. The electronic structure of the Ru site is regulated by the alloying effect with Co, optimizing the adsorption energy to *H and *OH and accelerating the HER/HOR kinetics. The RuCo/SANC NS catalyst exhibits excellent mass activity with HER of 13.58 A/mg Ru and HOR of 3.85 A/mg Ru , which are about 35.35 and 48.13 times that of Pt/C.
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
Science China-Materials
·
2025
·
IF 7.4
Zhang Tao,Wang Xin,Song Wanqing,Feng Jiahui,Yang Xinyi,Wang Haozhi,Ding Jia,Hu Wenbin
Alloying Pt with non-noble metals is effective for optimizing the activity of Pt-based electrocatalysts. However, the development of high-activity and stable hydrogen electrocatalysts remains challenging owing to the random elemental distribution and weak interatomic bonding in alloys. Herein, we reported a Pt 2 CoNi intermetallic nanocatalyst rich in surface microstrain for high-performance hydrogen electrocatalysis. The superlattice ordering crystalline structure ensures the specific positions of atoms in this nanocatalyst, resulting in the alternating arrangement of Pt and Co/Ni atoms. In one nanoparticle, multiple Pt 2 CoNi grains are arranged along different grain orientations, which generates abundant surface microstrain due to the discrepancy of intermetallic lattice parameters. The unique crystal structure effectively modulates the electron distribution of Pt 2 CoNi intermetallic nanocatalyst. The active sites of this nanocatalyst exhibit downshifted d-band centers, leading to accelerated hydrogen adsorption/desorption behavior. Resultantly, the Pt 2 CoNi intermetallic nanocatalyst demonstrates impressive bifunctional hydrogen electrocatalytic capabilities for hydrogen evolution reaction (mass activity of 1.02 A/mg Pt and η 10 variation of 3.7 mV after 10,000 cycles) and hydrogen oxidation reaction (kinetic mass activity of 4.08 A/mg Pt and 97.3% activity retention after 12 h operating at 0.1 V vs. RHE). This work provides a promising route for the development of efficient nanocatalysts with ingenious crystal structures.
研究领域:
纳米催化剂
·
电催化
·
材料科学
·
氢能
·
金属间化合物
✓ 已验证
产品关联
DOI
高影响因子
Nature Catalysis
·
2022
·Vol. 5
·期 10
·900-911
·
IF 40.706
Li Peng,Jiang Yaling,Hu Youcheng,Men Yana,Liu Yuwen,Cai Wenbin,Chen Shengli
The origin of the large kinetic pH effect in hydrogen electrocatalysis, that is, the approximately two orders of magnitude decrease in reaction kinetics when moving from acid to alkaline, remains far from having a consensus. Here we show that it is the significantly different connectivity of hydrogen-bond networks in electric double layers that causes the large kinetic pH effect. This result has been obtained by meticulously comparing the electric double layers of acid and alkaline interfaces from ab initio molecular dynamics simulations, and the computed vibrational density of states of water molecules in the interfaces simulated with ab initio molecular dynamics, with the results of in situ surface-enhanced infrared absorption spectroscopy. Using a Pt–Ru alloy as a model catalyst, we further reveal an unanticipated role of OH adsorption in improving the kinetics of alkaline hydrogen electrocatalysis, namely, by increasing the connectivity of hydrogen-bond networks in electric double layers rather than by merely affecting the energetics of surface reaction steps. These findings highlight the key roles of electric double layer structures in electrocatalysis.
研究领域:
电化学
·
催化
·
材料科学
·
表面科学
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Wuyi Feng,Jiantao Fu,Xinye Zheng,Wei Zhu,Zhongbin Zhuang,Di Zhao,Jiatao Zhang
Optimizing the intrinsic hydrogen binding energy at atomic-level interfaces is beneficial and challenging for hydrogen electrocatalysis to improve the mass activity of platinum-group metal. Here, we develop a bifunctional hydrogen electrocatalyst featuring atomically dispersed Rh-N 4 sites alongside ultrasmall Rh nanoparticles (Rh SA+NP /NC). For the hydroxide oxidation reaction, the mass activity (9.14 A mg Rh −1 ) of Rh SA+NP /NC is 101 times that of commercial Pt/C. For the hydrogen evolution reaction, the overpotential is merely 14 mV at an extremely low Rh loading (1.91 μg cm −2 ). The anion-exchange membrane fuel cell and anion-exchange membrane water electrolyzer equipped with Rh SA+NP /NC achieve a high peak power density (25.7 W mg Rh −1 ) and a low cell voltage (1.77 V at 1 A cm −2 ), respectively. Experimental and computational results indicate that the atomic-level interface formed by Rh single atoms and nanoparticles optimizes the adsorption behavior of active species and accelerates the hydrogen conversion kinetics. This study designs cost-effective hydrogen electrocatalysts through atomic-level interface engineering, providing a feasible strategy for accelerating the realization of a sustainable hydrogen circular economy.
研究领域:
电催化
·
材料科学
·
能量转换
·
纳米材料
·
氢能
✓ 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）