Small
·
2023
·Vol. 19
·期 41
·2302685
·
IF 13.3
Hancheng Ma,Xiang Huang,Luyu Li,Wei Peng,Sheng Lin,Yao Ding,Liqiang Mai
PtTe 2 , a member of the noble metal dichalcogenides (NMDs), has aroused great interest in exploring its behavior in the hydrogen evolution reaction (HER) due to the unique type-II topological semimetallic nature. In this work, a simple template-free hydrothermal method to obtain the phosphorus-doped (P-doped) PtTe 2 nanocages with abundant amorphous and crystalline interface (A/C-P-PtTe 2 ) is developed. Revealed by density functional theory calculations, the atomic Te vacancies can spontaneously form on the basal planes of PtTe 2 by the P doping, which results in the unsaturated Pt atoms exposed as the active sites in the amorphous layer for HER. Owing to the defective structure, the A/C-P-PtTe 2 catalysts have the fast Tafel step determined kinetics in HER, which contributes to an ultralow overpotential ( η = 28 mV at 10 mA cm −2 ) and a small Tafel slope of 37 mV dec −1 . More importantly, benefiting from the inner stable crystalline P-PtTe 2 nanosheets, limited decay of the performance is observed after chronopotentiometry test. This work reveals the important role of the inherent relationship between structure and activity in PtTe 2 for HER, which may bring another enlightenment for the design of efficient catalysts based on NMDs in the near future.
研究领域:
材料科学
·
电化学
·
纳米催化
·
能源材料
·
计算材料学
✓ 已验证
DOI
高影响因子
MATERIALS & DESIGN
·
2016
·
IF 3.997
XinRong Liu,Ming Zhang,TingTing Yang,LiNa Wang,Han Zhu,ShunLi Wang,MingLiang Du
Carbon nanofibers served as nanoreactors for the design and construction of PtCo alloy carbon core-shell nanostructures with nitrogen doping (PtCo/NCNF) through a combination of electrospinning and nitrogen doping treatments. The PtCo/NCNF hybrid consists of PtCo alloy nanoparticles surrounded by a few of N-doped carbon layers , demonstrating a typical core-shell structures. The PtCo/NCNF hybrid can both served as electrode materials for electrocatalytic water splitting including hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). For the HER performance, the PtCo/NCNF exhibits very small onset potential of 20 mV, an overpotential of 50 mV at a j (vs RHE) = 10 mA cm − 2 and Tafel slope of 30 mV dec − 1 . The PtCo/NCNF hybrid also exhibits high OER activity with an onset potential of 310 mV, an overpotential of 400 mV at a j of 10 mA cm − 2 and a small Tafel slope of 76 mV dec − 1 . The high catalytic activities of PtCo alloy for HER and OER originate from the 3D hierarchical structures, well-dispersed PtCo alloy, high conductivity of NCNF, protection from the carbon-encapsulated structure, and the introduction of nitrogen.
研究领域:
材料科学
·
纳米技术
·
电化学
·
能源化学
·
催化化学
·
功能材料
✓ 已验证
DOI
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2021
·Vol. 42
·期 10
·1798-1807
·
IF 8.271
Xiangyong Zhang,Tianying Liu,Ting Guo,Xueying Han,Zongyun Mu,Qiang Chen,Jiangmin Jiang,Jing Yan,Jiaren Yuan,Dezhi Wang,Zhuangzhi Wu,Zongkui Kou
Controllably mounting foreign atoms on the surfaces of earth-abundant electrocatalysts strongly improve their surface electronic properties for optimizing the catalytic performance of surficial sites to an unusual level, and provides a good platform to gain deep insights into catalytic reactions . The present work describes, employing ultrafine W 2 C nanoislands (average size: 2.3 nm) monodispersed on the N, P dual-doped carbon frameworks as a model system, how to regulate the atomic phosphorous-mounting effect on the surfaces of W 2 C to derive an active and stable P-mounting W 2 C (WCP) catalyst for both acidic and alkaline hydrogen evolution reaction (HER). Since in situ phosphorus substitution into carbon sites of preformed W 2 C nanoislands gradually proceeds from surfaces to solids, so that using a proper amount of phosphorus sources can readily control the surface mounting level to avoid the mass P-doping into the bulk. By this way, the activity per active site of WCP catalyst with robust stability can be optimized to 0.07 and 0.56 H 2 s −1 at –200 mV overpotential in acid and base, respectively, which reach up to the several-fold of pure-phase W 2 C (0.01 and 0.05 H 2 s −1 ). Theoretical investigations suggest that compared with solid P doping, the P mounting on W 2 C surface can more remarkably enhance its metallicity and decrease the hydrogen release barrier. This finding disclosed a key correlation between surface foreign atom-mounting and catalytic activity , and suggested a logical extension to other earth-abundant catalysts for various catalytic reactions .
研究领域:
材料化学
·
电催化
·
纳米材料
·
能源科学
·
表面科学
·
理论计算
✓ 已验证
DOI
高影响因子
ELECTROCHIMICA ACTA
·
2018
·
IF 5.116
Xiaozhen Chen,Ji Qi,Pan Wang,Chuang Li,Xiao Chen,Changhai Liang
Herein, PVA-Mo 2 C/Mo 2 N nanospheres with surface roughness are synthesized via a polyvinyl alcohol (PVA) involved approach and used for hydrogen evolution reaction (HER). The average crystallite size of the PVA protected nMo 2 CN nanospheres (6.1 nm) is one third of that of the PVA-Mo 2 C/Mo 2 N without PVA protection (17.9 nm). At 10 mA cm −2 current density, the as-synthesized PVA-Mo 2 C/Mo 2 N nanospheres with surface roughness exhibit HER overpotentials of 132 mV and 142 mV with corresponding Tafel slope of 51.8 mV dec −1 and 50.4 mV dec −1 in acid and alkaline medium, respectively. This high apparent activity can be attributed to the high intrinsic activity originated from the adjacent surface active sites of Mo 2 C and Mo 2 N as well as the large ECSA of PVA-Mo 2 C/Mo 2 N nanospheres with surface roughness.
研究领域:
材料科学
·
电化学
·
纳米催化
·
能源化学
·
表面科学
✓ 已验证
DOI
高影响因子
Small
·
2024
·Vol. 21
·期 4
·2410657
·
IF 13
Jia Wang,De Wang,Zelin Zhao,Ganggang Chang,Wei Guo,Jun Xu,Yinyu Xiang,Junrui Li,Junsheng Li
Developing cost-effective ruthenium (Ru)-based HER electrocatalysts as alternatives to commercial Pt/C is crucial for the advancement of proton exchange membrane water electrolysis (PEMWE). However, the strong hydrogen adsorption of Ru-based catalysts restricts its activity. Herein, a strategy is reported to tune the electronic structure and improve mass transfer by implanting Ru atoms onto the (002) facet of two-dimensional zeolitic imidazolate framework-67 (Ru@ L ZIF (002) ) to optimize the d -band center ( ε d ) of Ru and the hydrogen spillover behavior. Benefiting from the ultrathin nanosheet structure and optimized ε d of Ru, the over-strong H adsorption energy is weakened and the electron/mass transfer is facilitated. Ru@ L ZIF (002) exhibits an overpotential of 9.2 mV at 10 mA cm −2 and a long-lasting stability of 35 days at 100 mA cm −2 . The mass activity and price activity of Ru@ L ZIF (002) is 2.9 and 14.7 times higher than Pt/C, respectively. More impressively, Ru@ L ZIF (002) delivers a cell voltage of 2.01 V at a high current density of 4 A cm −2 in PEMWE. The excellent long-term durability of 1200 hours operating at 4 A cm −2 with an ultralow decay rate of 7.5 × 10 −3 mV h −1 has been achieved, making it promising as a cost-effective alternative to Pt/C catalyst for PEMWE applications.
研究领域:
电催化
·
材料科学
·
能源化学
·
纳米材料
·
电化学工程
·
可持续能源技术
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）