scholarly journals A fundamental viewpoint on the hydrogen spillover phenomenon of electrocatalytic hydrogen evolution

2021 ◽  
Vol 12 (1) ◽  
Author(s):  
Jiayuan Li ◽  
Jun Hu ◽  
Mingkai Zhang ◽  
Wangyan Gou ◽  
Sai Zhang ◽  
...  
Keyword(s):  
Hydrogen Evolution ◽  
Hydrogen Transfer ◽  
High Energy ◽  
Hydrogen Spillover ◽  
High Energy Barrier ◽  
Proton Adsorption ◽  
Work Function Difference ◽  
Supported Electrocatalysts ◽  
And Control ◽  
Interfacial Charge

AbstractHydrogen spillover phenomenon of metal-supported electrocatalysts can significantly impact their activity in hydrogen evolution reaction (HER). However, design of active electrocatalysts faces grand challenges due to the insufficient understandings on how to overcome this thermodynamically and kinetically adverse process. Here we theoretically profile that the interfacial charge accumulation induces by the large work function difference between metal and support (∆Φ) and sequentially strong interfacial proton adsorption construct a high energy barrier for hydrogen transfer. Theoretical simulations and control experiments rationalize that small ∆Φ induces interfacial charge dilution and relocation, thereby weakening interfacial proton adsorption and enabling efficient hydrogen spillover for HER. Experimentally, a series of Pt alloys-CoP catalysts with tailorable ∆Φ show a strong ∆Φ-dependent HER activity, in which PtIr/CoP with the smallest ∆Φ = 0.02 eV delivers the best HER performance. These findings have conclusively identified ∆Φ as the criterion in guiding the design of hydrogen spillover-based binary HER electrocatalysts.

scholarly journals A fundamental viewpoint on the hydrogen spillover phenomenon of electrocatalytic hydrogen evolution

2020 ◽  
Author(s):  
Jiayuan Li ◽  
Jun Hu ◽  
Mingkai Zhang ◽  
Wangyan Gou ◽  
Sai Zhang ◽  
...  
Keyword(s):  
Hydrogen Evolution ◽  
Hydrogen Transfer ◽  
High Energy ◽  
Hydrogen Spillover ◽  
High Energy Barrier ◽  
Proton Adsorption ◽  
Work Function Difference ◽  
Supported Electrocatalysts ◽  
And Control ◽  
Interfacial Charge

Abstract Hydrogen spillover phenomenon of metal-supported electrocatalysts can significantly impact their activity in hydrogen evolution reaction (HER). However, design of active electrocatalysts faces grand challenges due to the insufficient understandings on how to overcome this thermodynamically and kinetically adverse process. We theoretically profile that the interfacial charge accumulation induced by the large work function difference between metal and support (∆Φ) and sequentially strong interfacial proton adsorption construct a high energy barrier for hydrogen transfer. Theoretical simulations and control experiments rationalize that small ∆Φ induces interfacial charge dilution and relocation, thereby weakening interfacial proton adsorption and enabling efficient hydrogen spillover for HER. Experimentally, a series of Pt alloys-CoP catalysts with tailorable ∆Φ showed a strong ∆Φ-dependent HER activity, in which PtIr/CoP with the smallest ∆Φ = 0.02 eV delivered the best HER performance. These findings have conclusively identified ∆Φ as the criterion in guiding the design of hydrogen spillover-based binary HER electrocatalysts.

Electrochemical Behavior of Ni-based Alloys for Hydrogen Evolution Reaction in Alkaline Media

2012 ◽  
Vol 15 (3) ◽  
pp. 211-214
Author(s):  
Liliana Vazquez-Nava ◽  
Karina Patlán-Olmedo ◽  
Miguel A. Oliver-Tolentino ◽  
Rosa Gonzalez-Huerta ◽  
Hector J. Dorantes-Rosales ◽  
...  
Keyword(s):  
Hydrogen Evolution ◽  
Hydrogen Evolution Reaction ◽  
Open Circuit Potential ◽  
Linear Sweep Voltammetry ◽  
High Energy ◽  
Open Circuit ◽  
Alkaline Media ◽  
Tafel Slopes ◽  
Alkaline Conditions ◽  
Proton Adsorption

*Nickel-based alloys (Ni0.8CoO0.1Zn0.05MnO0.02Ti0.01Y0.01Al0.01(M1), NiO0.8CoO0.1Zn0.05MnO0.02Ti0.01Y0.01Al0.01 (M2) and NiO0.6CoO0.35Zn0.025Ti0.025 (M3)) were synthesized from high purity powders by means of high-energy mechanical milling. The hydrogen evolution reaction (HER) kinetic-performance of the as-prepared materials was evaluated using linear sweep voltammetry at alkaline conditions and room temperature. According to kinetic parameters calculated from Tafel slopes, the sample M2 showed the better activity in the HER. These results suggest that the electrode surface state in the material play an important role in the proton-adsorption kinetic as demonstrated by SEM, open circuit potential transients and cyclic voltammetry techniques.

Enhancing the energy barrier and hysteresis temperature in two benchtop-stable Ho(III) single-ion magnets

2021 ◽  
Author(s):  
Kexin Jia ◽  
Xixi Meng ◽  
Mengmeng Wang ◽  
Xiaoshuang Gou ◽  
Yu-Xia Wang ◽  
...  
Keyword(s):  
Energy Barrier ◽  
High Energy ◽  
Halogen Anion ◽  
High Energy Barrier

The energy barrier and hysteresis temperature in two benchtop-stable D5h-symmetry HoIII single-ion magnets were significantly enhanced via the variation of halogen anion. The coexistence of high energy barrier of 418...

scholarly journals Current Knowledge and Future Directions for Improving Subsoiling Quality and Reducing Energy Consumption in Conservation Fields

Agriculture ◽  
2021 ◽  
Vol 11 (7) ◽  
pp. 575
Author(s):  
Shangyi Lou ◽  
Jin He ◽  
Hongwen Li ◽  
Qingjie Wang ◽  
Caiyun Lu ◽  
...  
Keyword(s):  
Energy Consumption ◽  
Cover Crops ◽  
Current Knowledge ◽  
High Energy ◽  
Field Application ◽  
Research Progress ◽  
Monitoring And Control ◽  
Future Directions ◽  
Tillage Depth ◽  
And Control

Subsoiling has been acknowledged worldwide to break compacted hardpan, improve soil permeability and water storage capacity, and promote topsoil deepening and root growth. However, there exist certain factors which limit the wide in-field application of subsoiling machines. Of these factors, the main two are poor subsoiling quality and high energy consumption, especially the undesired tillage depth obtained in the field with cover crops. Based on the analysis of global adoption and benefits of subsoiling technology, and application status of subsoiling machines, this article reviewed the research methods, technical characteristics, and developing trends in five key aspects, including subsoiling shovel design, anti-drag technologies, technologies of tillage depth detection and control, and research on soil mechanical interaction. Combined with the research progress and application requirements of subsoiling machines across the globe, current problems and technical difficulties were analyzed and summarized. Aiming to solve these problems, improve subsoiling quality, and reduce energy consumption, this article proposed future directions for the development of subsoiling machines, including optimizing the soil model in computer simulation, strengthening research on the subsoiling mechanism and comprehensive effect, developing new tillage depth monitoring and control systems, and improving wear-resisting properties of subsoiling shovels.

scholarly journals Insights on forming N,O-coordinated Cu single-atom catalysts for electrochemical reduction CO2 to methane

2021 ◽  
Vol 12 (1) ◽  
Author(s):  
Yanming Cai ◽  
Jiaju Fu ◽  
Yang Zhou ◽  
Yu-Chung Chang ◽  
Qianhao Min ◽  
...  
Keyword(s):  
Energy Barrier ◽  
Active Sites ◽  
Theoretical Calculations ◽  
High Energy ◽  
Single Atom ◽  
Faradaic Efficiency ◽  
High Energy Barrier ◽  
Catalytic Sites ◽  
Electron Reduction ◽  
First Time

AbstractSingle-atom catalysts (SACs) are promising candidates to catalyze electrochemical CO2 reduction (ECR) due to maximized atomic utilization. However, products are usually limited to CO instead of hydrocarbons or oxygenates due to unfavorable high energy barrier for further electron transfer on synthesized single atom catalytic sites. Here we report a novel partial-carbonization strategy to modify the electronic structures of center atoms on SACs for lowering the overall endothermic energy of key intermediates. A carbon-dots-based SAC margined with unique CuN2O2 sites was synthesized for the first time. The introduction of oxygen ligands brings remarkably high Faradaic efficiency (78%) and selectivity (99% of ECR products) for electrochemical converting CO2 to CH4 with current density of 40 mA·cm-2 in aqueous electrolytes, surpassing most reported SACs which stop at two-electron reduction. Theoretical calculations further revealed that the high selectivity and activity on CuN2O2 active sites are due to the proper elevated CH4 and H2 energy barrier and fine-tuned electronic structure of Cu active sites.

Slow magnetic relaxation in dinuclear dysprosium and holmium phenoxide bridged complexes: a Dy2 single molecule magnet with a high energy barrier

2021 ◽  
Author(s):  
Matilde Fondo ◽  
Julio Corredoira-Vázquez ◽  
Ana M. Garcia-Deibe ◽  
Jesus Sanmartin Matalobos ◽  
Silvia Gómez-Coca ◽  
...  
Keyword(s):  
Crystal Structures ◽  
Single Molecule ◽  
Energy Barrier ◽  
Magnetic Relaxation ◽  
High Energy ◽  
Single Molecule Magnet ◽  
High Energy Barrier ◽  
Slow Magnetic Relaxation

Dinuclear [M(H3L1,2,4)]2 (M = Dy, Dy2; M = Ho, Ho2) complexes were isolated from an heptadentate aminophenol ligand. The crystal structures of Dy2·2THF, and the pyridine adducts Dy2·2Py and Ho2·2Py,...

scholarly journals Overfeeding Extends the Period of Annual Cyclicity but Increases the Risk of Early Embryonic Death in Shetland Pony Mares

Animals ◽  
2021 ◽  
Vol 11 (2) ◽  
pp. 361
Author(s):  
Nicky M. M. D’Fonseca ◽  
Charlotte M. E. Gibson ◽  
Iris Hummel ◽  
David A. van Doorn ◽  
Ellen Roelfsema ◽  
...  
Keyword(s):  
Embryo Transfer ◽  
Reproductive Activity ◽  
High Energy ◽  
Morphometric Parameters ◽  
Net Energy ◽  
Conceptus Development ◽  
And Control ◽  
Annual Duration ◽  
Embryonic Death

Obesity has been associated with altered reproductive activity in mares, and may negatively affect fertility. To examine the influence of long-term high-energy (HE) feeding on fertility, Shetland pony mares were fed a diet containing 200% of net energy (NE) requirements during a three-year study. The incidence of hemorrhagic anovulatory follicles (HAF) and annual duration of cyclicity were compared to those in control mares receiving a maintenance diet. Day-7 embryos were flushed and transferred between donor and recipient mares from both groups; the resulting conceptuses were collected 21 days after transfer to assess conceptus development. HE mares became obese, and embryos recovered from HE mares were more likely to succumb to early embryonic death. The period of annual cyclicity was extended in HE compared to control mares in all years. The incidence of HAFs did not consistently differ between HE and control mares. No differences in embryo morphometric parameters were apparent. In conclusion, consuming a HE diet extended the duration of cyclicity, and appeared to increase the likelihood of embryos undergoing early embryonic death following embryo transfer.

Reduced substrate oxidation in postischemic myocardium: 13C and 31P NMR analyses

1990 ◽  
Vol 258 (5) ◽  
pp. H1357-H1365 ◽  
Author(s):  
E. D. Lewandowski ◽  
D. L. Johnston
Keyword(s):  
Steady State ◽  
31P Nmr ◽  
Tca Cycle ◽  
High Energy ◽  
Substrate Oxidation ◽  
High Energy Phosphates ◽  
Atp Content ◽  
And Control ◽  
13C And 31P Nmr ◽  
Postischemic Myocardium

13C and 31P nuclear magnetic resonance (NMR) spectra were used to assess substrate oxidation and high-energy phosphates in postischemic (PI) isolated rabbit hearts. Phosphocreatine (PCr) increased in nonischemic controls on switching from glucose perfusion to either 2.5 mM [3-13C]pyruvate (120%, n = 7) or [2-13C]acetate (114%, n = 8, P less than 0.05). ATP content, oxygen consumption (MVO2), and hemodynamics (dP/dt) were not affected by substrate availability in control or PI hearts. dP/dt was 40-60% lower in PI hearts during reperfusion after 10 min ischemia. Hearts reperfused with either pyruvate (n = 11) or acetate (n = 8) regained preischemic PCr levels within 45 s. Steady-state ATP levels were 55-70% of preischemia with pyruvate and 52-60% with acetate. Percent maximum [4-13C]glutamate signal showed reduced conversion of pyruvate to glutamate via the tricarboxylic acid (TCA) cycle at 4-min reperfusion (PI = 24 +/- 4%, means +/- SE; Control = 48 +/- 4%). The increase in 13C signal from the C-4 position of glutamate was similar to control hearts within 10.5 min. The increase in [4-13C]glutamate signal from acetate was not different between PI and control hearts. The ratio of [2-13C]Glu:[4-13C]Glu, reflecting TCA cycle activity, was reduced in PI hearts with acetate for at least 10 min (Control = 0.76 +/- 0.03; PI = 0.51 +/- 0.09) until steady state was reached. Despite rapid recovery of oxidative phosphorylation, contractility remained impaired and substrate oxidation was significantly slowed in postischemic hearts.

First principle simulation on oxidation mechanism of diethyl ether by nitrogen dioxide

2015 ◽  
Vol 14 (03) ◽  
pp. 1550020 ◽  
Author(s):  
Yuan Yuan ◽  
Wei Hu ◽  
Xuhui Chi ◽  
Cuihua Li ◽  
Dayong Gui ◽  
...  
Keyword(s):  
Diethyl Ether ◽  
Energy Barrier ◽  
Density Functional ◽  
Oxidation Process ◽  
Oxidation Mechanism ◽  
High Energy ◽  
First Principle ◽  
Functional Theory ◽  
The Third ◽  
High Energy Barrier

The oxidation mechanism of diethyl ethers by NO2was carried out using density functional theory (DFT) at the B3LYP/6-31+G (d, p) level. The oxidation process of ether follows four steps. First, the diethyl ether reacts with NO2to produce HNO2and diethyl ether radical with an energy barrier of 20.62 kcal ⋅ mol-1. Then, the diethyl ether radical formed in the first step directly combines with NO2to form CH3CH ( ONO ) OCH2CH3. In the third step, the CH3CH ( ONO ) OCH2CH3was further decomposed into the CH3CH2ONO and CH3CHO with a moderately high energy barrier of 32.87 kcal ⋅ mol-1. Finally, the CH3CH2ONO continues to react with NO2to yield CH3CHO , HNO2and NO with an energy barrier of 28.13 kcal ⋅ mol-1. The calculated oxidation mechanism agrees well with Nishiguchi and Okamoto's experiment and proposal.

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