2,2’-Dipyridylamine as Organic Molecular Electrocatalyst for Hydrogen Evolution Reaction in Acidic Electrolytes

2019 ◽  
Author(s):  
Xi Yin ◽  
Ling Lin ◽  
Hoon T. Chung ◽  
Ulises Martinez ◽  
Andrew M. Baker ◽  
...  
Keyword(s):  
Hydrogen Evolution ◽  
Hydrogen Evolution Reaction ◽  
Density Functional ◽  
Low Cost ◽  
Membrane Electrode Assembly ◽  
Carbon Surface ◽  
Membrane Electrode ◽  
Durability Test ◽  
Onset Potential ◽  
Precious Metal Catalysts

Finding a low-cost and stable electrocatalyst for hydrogen evolution reaction (HER) as a replacement for scarce and expensive precious metal catalysts has attracted significant interest from chemical and materials research communities. Here, we demonstrate an organic catalyst based on 2,2’-dipyridylamine (dpa) molecules adsorbed on carbon surface, which shows remarkable hydrogen evolution activity and performance durability in strongly acidic polymer electrolytes without involving any metal. The HER onset potential at dpa adsorbed on carbon has been found to be less than 50 mV in sulfuric acid and in a Nafion-based membrane electrode assembly (MEA). At the same time, this catalyst has shown no performance loss in a 60-hour durability test. The HER reaction mechanisms and the low onset overpotential in this system are revealed based on electrochemical study. Density functional theory (DFT) calculations suggest that the pyridyl-N functions as the active site for H adsorption with a free energy of -0.13 eV, in agreement with the unusually low onset overpotential for an organic molecular catalyst.<br>

2,2’-Dipyridylamine as Organic Molecular Electrocatalyst for Hydrogen Evolution Reaction in Acidic Electrolytes

2019 ◽  
Author(s):  
Xi Yin ◽  
Ling Lin ◽  
Hoon T. Chung ◽  
Ulises Martinez ◽  
Andrew M. Baker ◽  
...  
Keyword(s):  
Hydrogen Evolution ◽  
Hydrogen Evolution Reaction ◽  
Density Functional ◽  
Low Cost ◽  
Membrane Electrode Assembly ◽  
Carbon Surface ◽  
Membrane Electrode ◽  
Durability Test ◽  
Onset Potential ◽  
Precious Metal Catalysts

Finding a low-cost and stable electrocatalyst for hydrogen evolution reaction (HER) as a replacement for scarce and expensive precious metal catalysts has attracted significant interest from chemical and materials research communities. Here, we demonstrate an organic catalyst based on 2,2’-dipyridylamine (dpa) molecules adsorbed on carbon surface, which shows remarkable hydrogen evolution activity and performance durability in strongly acidic polymer electrolytes without involving any metal. The HER onset potential at dpa adsorbed on carbon has been found to be less than 50 mV in sulfuric acid and in a Nafion-based membrane electrode assembly (MEA). At the same time, this catalyst has shown no performance loss in a 60-hour durability test. The HER reaction mechanisms and the low onset overpotential in this system are revealed based on electrochemical study. Density functional theory (DFT) calculations suggest that the pyridyl-N functions as the active site for H adsorption with a free energy of -0.13 eV, in agreement with the unusually low onset overpotential for an organic molecular catalyst.<br>

Tuning the Edge-Site Activity of 2H Phase MoSe2 for Hydrogen Evolution Reaction via Sulfur Substitution and Strain Engineering

2020 ◽  
Vol 12 (10) ◽  
pp. 1446-1456
Author(s):  
Ziwei Xu ◽  
Guanghui Zhao ◽  
Mingyuan Wang ◽  
Jingjing Liang ◽  
Shahid Hussain ◽  
...  
Keyword(s):  
Catalytic Activity ◽  
Hydrogen Evolution ◽  
Hydrogen Evolution Reaction ◽  
Density Functional ◽  
High Efficiency ◽  
Low Cost ◽  
Catalytic Efficiency ◽  
Strain Engineering ◽  
Catalyst Design ◽  
Potential Candidate

The 2H phase MoSe2 of high chemical stability and excellent catalytic activity is a promising catalyst for the hydrogen evolution reaction (HER) as a potential candidate, due to its low cost, high efficiency and abundant production. However, the HER catalytic efficiency of MoSe2 largely depends on the activity of reaction sites including the basal plane and the edges, and remains low because only the Mo edge sites are active. Herein, we have calculated the structural stability, catalytic activity, and strain engineering on sulfur substituted MoSe2 catalytic structures (Mo(Se1–xSx)2) by density functional theory. The results demonstrate that most of Mo(Se1–xSx)2 monolayers are thermodynamically stable and the HER activity of the Mo(Se1–xSx)2 monolayers can be effectively tuned by both element substitution and strain engineering with the mechanisms uncovered at the atomic level. This study provides the experiments theoretical references for the novel catalyst design of the hydrogen evolution reaction.

scholarly journals Ultra-small hollow ternary alloy nanoparticles for efficient hydrogen evolution reaction

2020 ◽  
Author(s):  
Zhenxing Li ◽  
Chengcheng Yu ◽  
Yikun Kang ◽  
Xin Zhang ◽  
Yangyang Wen ◽  
...  
Keyword(s):  
Hydrogen Evolution ◽  
Ternary Alloy ◽  
Hydrogen Evolution Reaction ◽  
Density Functional ◽  
Low Cost ◽  
Average Diameter ◽  
One Pot ◽  
Design And Synthesis ◽  
Hollow Structures ◽  
New Strategy

Abstract Hollow nanoparticles with large specific surface area and high atom utilization are promising catalysts for the hydrogen evolution reaction (HER). We describe herein the design and synthesis of a series of ultra-small hollow ternary alloy nanostructures using a simple one-pot strategy. The same technique was demonstrated for hollow PtNiCu nanoparticles, hollow PtCoCu nanoparticles, and hollow CuNiCo nanoparticles. During synthesis, the displacement reaction and oxidative etching played important roles in the formation of hollow structures. Moreover, our hollow PtNiCu and PtCoCu nanoparticles were single-crystalline, with an average diameter of 5 nm. Impressively, ultra-small hollow PtNiCu nanoparticles, containing only 10% Pt, exhibited greater electrocatalytic HER activity and stability than a commercial Pt/C catalyst. The overpotential of hollow PtNiCu nanoparticles at 10 mA cm−2 was 28 mV versus RHE. The mass activity was 4.54 A mgPt−1 at -70 mV versus RHE, which is 5.62-fold greater than that of a commercial Pt/C system (0.81 A mgPt−1). Through analyses of bonding and antibonding orbital filling, density functional theory (DFT) calculations demonstrated that the bonding strength of different metals to the hydrogen intermediate (H*) was in the order of Pt &gt; Co &gt; Ni &gt; Cu. The excellent HER performance of our hollow PtNiCu nanoparticles derives from moderately synergistic interactions between the three metals and H*. This work demonstrates a new strategy for the design of low-cost and high-activity HER catalysts.

scholarly journals Designing electrolyte structure to suppress hydrogen evolution reaction in aqueous batteries

2020 ◽  
Author(s):  
Qingshun Nian ◽  
Xiaoren Zhang ◽  
Yazhi Feng ◽  
Shuang Liu ◽  
Tianjiang Sun ◽  
...  
Keyword(s):  
Hydrogen Evolution ◽  
Hydrogen Evolution Reaction ◽  
Low Cost ◽  
Dynamics Simulation ◽  
Anode Surface ◽  
Hydrogen Bond Acceptor ◽  
Onset Potential ◽  
Electrochemical Window ◽  
Novel Design ◽  
Aqueous Batteries

Abstract Aqueous batteries (ABs) have attracted increasing attention because of their inherent safety and low cost. Nevertheless, hydrogen evolution reaction (HER) at the anode presents severe challenges for stable and safe operation of ABs. Instead of passivating the anode surface to hinder HER kinetics, a novel design strategy is proposed here to suppress the HER via alternating its thermodynamics pathway. By adding a hydrogen bond acceptor, dimethyl sulfoxide (DMSO), the onset potential of HER can be delayed by as much as 1.0 V (on titanium mesh). Spectral characterization and molecular dynamics simulation confirm that the formation of hydrogen bonds between DMSO and water molecules can reduce the water activity, thereby suppressing the HER. This strategy has proven to be universal in expanding the electrochemical window of aqueous electrolytes. For instance, unconventional V2+↔V3+ redox processes in Na3V2(PO4)3 (-1.2 V versus Ag/AgCl) and highly stable Zn plating/stripping processes can be realized in ABs.

scholarly journals Wittichenite semiconductor of Cu3BiS3 films for efficient hydrogen evolution from solar driven photoelectrochemical water splitting

2021 ◽  
Vol 12 (1) ◽  
Author(s):  
Dingwang Huang ◽  
Lintao Li ◽  
Kang Wang ◽  
Yan Li ◽  
Kuang Feng ◽  
...  
Keyword(s):  
Hydrogen Evolution ◽  
Water Splitting ◽  
Low Cost ◽  
Solar Hydrogen ◽  
Onset Potential ◽  
Term Stability ◽  
Long Term Stability ◽  
Solar Water Splitting ◽  
Current Densities

AbstractA highly efficient, low-cost and environmentally friendly photocathode with long-term stability is the goal of practical solar hydrogen evolution applications. Here, we found that the Cu3BiS3 film-based photocathode meets the abovementioned requirements. The Cu3BiS3-based photocathode presents a remarkable onset potential over 0.9 VRHE with excellent photoelectrochemical current densities (~7 mA/cm2 under 0 VRHE) and appreciable 10-hour long-term stability in neutral water solutions. This high onset potential of the Cu3BiS3-based photocathode directly results in a good unbiased operating photocurrent of ~1.6 mA/cm2 assisted by the BiVO4 photoanode. A tandem device of Cu3BiS3-BiVO4 with an unbiased solar-to-hydrogen conversion efficiency of 2.04% is presented. This tandem device also presents high stability over 20 hours. Ultimately, a 5 × 5 cm2 large Cu3BiS3-BiVO4 tandem device module is fabricated for standalone overall solar water splitting with a long-term stability of 60 hours.

scholarly journals A monodispersed CuPt alloy: synthesis and its superior catalytic performance in the hydrogen evolution reaction over a full pH range

RSC Advances ◽  
2021 ◽  
Vol 11 (21) ◽  
pp. 12470-12475
Author(s):  
Xinmei Liu ◽  
Chen Liang ◽  
Wenlong Yang ◽  
Chunyang Yang ◽  
Jiaqi Lin ◽  
...  
Keyword(s):  
Hydrogen Evolution ◽  
Hydrogen Evolution Reaction ◽  
High Stability ◽  
Low Cost ◽  
Catalytic Performance ◽  
Ph Range

An effective approach to achieve the low cost and high stability of electro-catalysts for HER.

scholarly journals Engineering single-atomic ruthenium catalytic sites on defective nickel-iron layered double hydroxide for overall water splitting

2021 ◽  
Vol 12 (1) ◽  
Author(s):  
Panlong Zhai ◽  
Mingyue Xia ◽  
Yunzhen Wu ◽  
Guanghui Zhang ◽  
Junfeng Gao ◽  
...  
Keyword(s):  
Hydrogen Evolution ◽  
Water Splitting ◽  
Layered Double Hydroxide ◽  
Hydrogen Evolution Reaction ◽  
Active Sites ◽  
Density Functional ◽  
Rational Design ◽  
Single Atom ◽  
Nickel Iron ◽  
Double Hydroxide

AbstractRational design of single atom catalyst is critical for efficient sustainable energy conversion. However, the atomic-level control of active sites is essential for electrocatalytic materials in alkaline electrolyte. Moreover, well-defined surface structures lead to in-depth understanding of catalytic mechanisms. Herein, we report a single-atomic-site ruthenium stabilized on defective nickel-iron layered double hydroxide nanosheets (Ru1/D-NiFe LDH). Under precise regulation of local coordination environments of catalytically active sites and the existence of the defects, Ru1/D-NiFe LDH delivers an ultralow overpotential of 18 mV at 10 mA cm−2 for hydrogen evolution reaction, surpassing the commercial Pt/C catalyst. Density functional theory calculations reveal that Ru1/D-NiFe LDH optimizes the adsorption energies of intermediates for hydrogen evolution reaction and promotes the O–O coupling at a Ru–O active site for oxygen evolution reaction. The Ru1/D-NiFe LDH as an ideal model reveals superior water splitting performance with potential for the development of promising water-alkali electrocatalysts.

scholarly journals Modulating electronic structure of metal-organic frameworks by introducing atomically dispersed Ru for efficient hydrogen evolution

2021 ◽  
Vol 12 (1) ◽  
Author(s):  
Yamei Sun ◽  
Ziqian Xue ◽  
Qinglin Liu ◽  
Yaling Jia ◽  
Yinle Li ◽  
...  
Keyword(s):  
Electronic Structure ◽  
Hydrogen Evolution ◽  
Hydrogen Evolution Reaction ◽  
Density Functional ◽  
Metal Organic Frameworks ◽  
Catalyst Design ◽  
Single Atom ◽  
Hydrogen Energy ◽  
Structure Of Metal ◽  
Metal Organic

AbstractDeveloping high-performance electrocatalysts toward hydrogen evolution reaction is important for clean and sustainable hydrogen energy, yet still challenging. Herein, we report a single-atom strategy to construct excellent metal-organic frameworks (MOFs) hydrogen evolution reaction electrocatalyst (NiRu0.13-BDC) by introducing atomically dispersed Ru. Significantly, the obtained NiRu0.13-BDC exhibits outstanding hydrogen evolution activity in all pH, especially with a low overpotential of 36 mV at a current density of 10 mA cm−2 in 1 M phosphate buffered saline solution, which is comparable to commercial Pt/C. X-ray absorption fine structures and the density functional theory calculations reveal that introducing Ru single-atom can modulate electronic structure of metal center in the MOF, leading to the optimization of binding strength for H2O and H*, and the enhancement of HER performance. This work establishes single-atom strategy as an efficient approach to modulate electronic structure of MOFs for catalyst design.

Strategies on regulating Zn2+ solvation structure for dendrites-free and side reactions-suppressed zinc-ion batteries

2022 ◽  
Author(s):  
Jin Cao ◽  
Dongdong Zhang ◽  
Xinyu Zhang ◽  
Zhiyuan Zeng ◽  
Jiaqian Qin ◽  
...  
Keyword(s):  
Energy Storage ◽  
Hydrogen Evolution ◽  
Hydrogen Evolution Reaction ◽  
Low Cost ◽  
Zinc Ion ◽  
Side Reactions ◽  
Solvation Structure ◽  
Dendrites Growth

High‐safety and low‐cost aqueous zinc‐ion batteries (ZIBs) are an exceptionally compelling technology for grid‐scale energy storage, whereas the corrosion, hydrogen evolution reaction and dendrites growth of Zn anodes plague their...

scholarly journals Comprehensive Evaluation of Transition Metal Doped Ni3N to Construct High-Efficiency Hydrogen Evolution Catalyst

2021 ◽  
Author(s):  
Meng Wang ◽  
Zepeng Lv ◽  
Xuewei Lv ◽  
Qian Li ◽  
Jie Dang
Keyword(s):  
Transition Metal ◽  
Hydrogen Evolution ◽  
Density Functional ◽  
Rational Design ◽  
Dft Calculation ◽  
High Efficiency ◽  
Comprehensive Evaluation ◽  
Low Cost ◽  
Alkaline Electrolyte ◽  
Metal Doped

Abstract Density functional theory (DFT) calculation indicators (ΔG, densities of state, D-band and bader charge) are commonly used to predict and analyze the hydrogen evolution reaction (HER) activity of catalysts, and most studies discuss only one or few of these indicators’ impact on catalysis, but still no report has comprehensively evaluated the influence of all these indicators on catalytic performance. Herein, foreseen by comprehensive consideration first, we report transition metal doped Ni3N nanosheets combined on Ni foam for utra-efficient alkaline hydrogen evolution. For dual transition metals doped Ni3N, Co,V-Ni3N exhibits remarkable HER performance with a significantly low overpotential of only 10 mV in alkaline electrolyte and 41 mV in alkaline seawater electrolyte at 10 mA cm− 2; while for single transition metal doped Ni3N, V-Ni3N exhibits the best performance with an overpotential of 15 mV and a Tafel slope of 37 mV dec− 1. Our work highlights the importance of comprehensive evaluation of DFT calculation indexes, and opens up a new method for the rational design of efficient and low-cost catalysts.

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