ACS Applied Materials & Interfaces
·
2020
·
IF 8.758
Aleksei Chalgin,Wenlong Chen,Qian Xiang,Yi Wu,Fan Li,Fenglei Shi,Chengyi Song,Peng Tao,Wen Shang,Jianbo Wu
The urgent need of catalysts with improved performances toward the hydrogen evolution reaction (HER) is still one of the crucial issues for the water splitting electrocatalysis. Herein, we exhibit that the HER activity of the Pd nanocubes could be improved by selecting the appropriately shaped titania nanocrystals as support. In particular, we used Pd nanoparticles with (100)-facet exposed to show that the HER performance of Pd cubes can be improved in both acidic and alkaline electrolyte media when combined on the anatase TiO2 nanocrystals. Furthermore, we have also investigated the facet effect of TiO2 on the performance in detail, which indicated stronger catalytic activity when (001)-TiO2 was used rather than (mix 101/001)-TiO2 and (101)-TiO2. The electron-transfer-induced improvement of HER activity of Pd/TiO2 was assessed by electron energy loss spectroscopy (EELS). Thereafter, the combined support materials with suitable facet exposed can give an additional adjusting path to regulate the HER activities of Pd nanocatalysts, which henceforth can further contribute to a novel way for tuning other catalysts with good electrocatalytic properties.
研究领域:
材料科学
·
电化学
·
纳米技术
·
催化
✓ 已验证
DOI
高影响因子
ELECTROCHIMICA ACTA
·
2025
·
IF 5.6
Tinglei Huang,Beier Peng,Yuandi Zeng,Zhao Lu,Yufen Hu,Min Chen
The zinc anode in alkaline Zn-MnO 2 primary batteries suffers from high reactivity causing passivation, corrosion and low active-material utilization, affecting performance and durability. Herein, we introduce mannitol, a hydroxyl-rich organic molecule, as a dual-functional electrolyte additive to simultaneously optimize the solvation structure and suppress zinc corrosion in alkaline Zn-MnO 2 batteries. Theoretical calculations and experimental analyses reveal that the hydroxyl moieties in mannitol disrupt the original hydrogen-bond network, elevate the energy barrier of the hydrogen evolution reaction (HER), and mitigate parasitic water splitting. Concurrently, mannitol enhances interfacial corrosion resistance via chemisorption on the zinc anode surface and promotes the formation of a complex and dense passivation layer. The optimized electrolyte delivers a 12.3% increase in discharge capacity at 10 mA (25°C), with a corresponding rise in Zn utilization from 55.6% to 62.5%. Furthermore, significantly greater capacity improvements are observed under extreme temperatures: 17.4% at 80°C and 44.4% at -10°C. Additionally, the corrosion efficiency is reduced by 29.6% compared to the blank sample. This study deciphers the mechanism by which polyhydroxy organic molecules optimize the performance of alkaline aqueous batteries through modulating solvation structures and the electrode/electrolyte interface, offering a scalable strategy toward high-performance alkaline Zn-MnO 2 batteries.
研究领域:
电化学
·
储能
·
材料科学
·
电池技术
·
表面化学
✓ 已验证
产品关联
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2025
·
IF 19
Huimin Zhang,LinKe Guo,Jiaqi Liu,Xiaoyan Guo,Yanxin Ning,Xuning Wang,Dong Cao,Daojian Cheng
Generally fabricating single-atom alloys (SAAs) remains a major challenge. Herein, a SAAs library of PdM 1 (M = Os, Ir, Pt, Au, Pb, and Bi) is constructed and uncovered a volcano-type relationship between hydrogen evolution reaction (HER) activity and hydrogen binding energy (HBE). Remarkably, PdPt 1 SAAs, located at the top of the volcano plot, only require 10 mV at 10 mA cm −2 and exhibit 32.9 times higher intrinsic activity than commercial Pt/C in acidic condition. Moreover, PdPt 1 SAAs assembled in the proton exchange membrane water electrolyzer can maintain superior durability over 1000 h under the industrial current density of 1500 mA cm −2 . In situ spectroscopy measurements show PdPt 1 SAAs with moderate HBE display the fastest hydrogen adsorption and desorption kinetics in the SAAs library. Further theoretical calculations reveal PdPt 1 SAAs exhibit a moderate d -band center value, which leads to an optimal Pt─H bond strength and thus significantly lowers the Tafel step barrier during acidic HER. Finally, this approach is extended to prepare the other five additional binary, ternary, and high-entropy Pd-based SAAs.
研究领域:
催化
·
材料科学
·
电化学
·
能量转换
·
纳米材料
✓ 已验证
产品关联
DOI
高影响因子
Nanoscale
·
2024
·Vol. 16
·期 7
·3474-3483
·
IF 5.8
Yilin Wang,Xiao Chen,Yunmei Du,Shuangshuang Li,Mengmeng Wang,Yu Yang,Lei Wang
Simplifying the anchoring process of Ru nanoparticles (NPs) and activating their bifunctional activity are challenges in the construction of Ru-based catalysts. In this work, FeCoP nanosheets anchored by Ru NPs (r-Ru/FeCoP) were innovatively synthesized using an oxygen defect-assisted-gas-phase phosphorization strategy. Surprisingly, the η100 values of r-Ru/FeCoP in the alkaline hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) processes were 0.8 and 0.58 times those of Pt/C and RuO2, respectively. Notably, the rich Ru NPs as HER active sites on r-Ru/FeCoP enhanced the conductivity of the catalyst and promoted the reaction kinetics for HER, while the metal atoms on the FeCoP nanosheets served as OER active sites to accelerate the desorption of O2. The synergy between the two promoted the improvement of overall water splitting efficiency. Overall, this work provides a new approach for the development of low-cost bifunctional catalysts with high Ru utilization.
研究领域:
材料科学
·
催化
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Yan Liu,Liwen Xing,Yaqi Liu,Dianxing Lian,Mohaoyang Chen,Weiwei Zhang,Ke Wu,Hongdan Zhu,Zhiyi Sun,Wenxing Chen,Peng Wu,Dingsheng Wang,Yongjun Ji
The intrinsic activity of single-atom catalysts is influenced by the local electronic structures of metal centers, with existing modulation strategies limited to adjacent atomic coordination. However, the impacts of support surface geometry on local bonding environment, and thus electronic structures of single-atom centers have rarely been known. Here, we prepared highly curved B,N co-doped carbon-supported ruthenium catalyst with an ultra-low Ru loading of 0.4 wt%, which exhibited an ultrahigh turnover frequency (TOF) of 10 H 2 s −1 (38 times that of Pt/C) and superior stability in alkaline hydrogen evolution reaction (HER). We found that curving support surface induced the strain, resulting in 1.5% compressed Ru-N and 4% stretched Ru-B bonds, leading to the accumulation of positive charge and quenching of spin polarization at Ru sites, thereby achieving the optimal binding of H* and enhanced performance for HER. This work highlights the significant support effects upon the structural design of active sites.
研究领域:
催化
·
材料科学
·
化学
·
能源科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2018
·
IF 5.091
Yaqing Yin,Tingting Liu,Dan Liu,Zhao Wang,Qibo Deng,Deyu Qu,Zhizhong Xie,Haolin Tang,Junsheng Li
Despite recent progress in the development of earth abundant electrochemical catalyst for hydrogen evolution reaction (HER), Pt based materials still stand as the state of the art HER catalyst. Due to the high cost of Pt, it is desirable to increase the utilization efficiency of Pt in practical HER process to a realize cost effective hydrogen production . Herein, we repot a novel nitrogen doped ordered mesoporous carbon supported Pt (Pt@NOMC-A) catalyst with a low Pt loading of 7.2 wt% and show that the synergy between Pt nanoparticles and carbon support, as well as the physical confinement offered by the carbon support enhance the electrochemical performance of the novel catalyst. Pt@NOMC-A exhibits a low HER overpotential comparable with commercial 20 wt% Pt/C catalyst under acidic, neutral and alkaline condition. Furthermore, Pt@NOMC-A shows a superior electrochemical stability under working conditions suppressing that of commercial Pt/C catalyst.
研究领域:
材料科学
·
电化学
·
能源材料
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF CATALYSIS
·
2019
·
IF 7.723
Zuohui Wang,Nannan Heng,Xiaobing Wang,Jinling He,Yong Zhao
The original active site units and morphologies structure on catalyst surface is highly important to promote the rate of chemical reaction, while less concern is paid on their dynamic change during reaction process. Understanding these reconstructions in reactions is essential to illustrate the correlations between the structure and reactivity of catalyst, as well as the rational design of efficient catalyst. Here, single metal phophide materials are adopted as model electrocatalysts to show the structure evolution in the process of oxygen evolution reaction (OER) and hydrogen evolution reaction (HER). After both OER and HER operation, the core-shell structured metal-hydroxide/oxyhydroxide@metal-phosphide catalysts are generated, resulting in the high but decreased activity. To overcome the activity deterioration of metal phosphide induced by morphology reconstruction, binary heterostructure metal phosphides catalysts are designed and show the better OER and HER activity and stability compared to those of single phosphides. The work illustrates the structure-performance relationship of catalyst surface dynamics on catalytic performance, which will provide the guidance for designing high performance electrocatalysts, photocatalysts, and thermal catalysts.
研究领域:
电化学
·
催化
·
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Ze-Feng Xu,Chuan-Wu Chen,Ya-Nan Jing,Da-Qiang Liu,Hong-Xin Zhang,Qiu-Xia Lin,Lei-Lei Li,Xing-Liang Yin
Slow kinetics of the oxygen evolution reaction (OER) during water electrolysis limits hydrogen evolution reaction (HER) efficiency. Urea oxidation reaction (UOR), with a lower thermodynamic potential (0.37 V vs. RHE) than OER, offers an energy-saving alternative. Designing robust, multifunctional electrocatalysts for hydrogen generation by water electrolysis remains challenging. In this work, a universal two-stage solvothermal strategy was developed to synthesize α/β-FeOOH-based self-supported hierarchical structure catalysts on arbitrary metal substrates, evading polymeric binders. FeOOH/Fe achieves exceptional HER performance, while FeOOH/Ni delivers superior OER/UOR activity, exhibiting extremely-low UOR kinetics with a 12.24 mV·dec −1 Tafel slope. Asymmetric FeOOH/Ni (+)||FeOOH/Fe (−) electrolyzer requires ultralow voltages of 1.799 V (1.0 M KOH), 1.888 V (seawater/1.0 M KOH), and 1.627 V (0.33 M urea/1.0 M KOH) to drive 300 mA cm −2 , surpassing most similar systems. It maintains >9 Faraday efficiency over 100-h at ≥ 300 mA cm −2 , demonstrating industrial-grade stability. The catalysts’ accessible active sites, accelerated charge transfer, rapid kinetics, and superhydrophilicity synergistically enable rapid mass/electron transport and durable operation. This work provides a scalable platform for binder-free electrocatalysts, advancing practical hydrogen production through urea-assisted electrolysis and seawater utilization.
研究领域:
材料科学
·
电化学
·
可再生能源
✓ 已验证
产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Ying Wu,Min Li,Wenhui Fang,Yutao Cao,Shixian Xin,Hong Zhao
Electrochemical water splitting is a promising method for hydrogen production but is restricted by sluggish oxygen evolution reaction (OER), so we propose to replace OER with the thermodynamically preferred glucose oxidation reaction (GOR) to reduce the supply voltage. Herein, hollow RuV-Co(OH) 2 arrays have been fabricated by the hydrothermal method of sacrificing ZIF-67 to codope vanadium (V) and ruthenium (Ru). Electrochemical studies show that RuV-Co(OH) 2 has excellent hydrogen evolution reaction (HER) activity with a low overpotential of 77 mV at the current density of 10 mA cm −2 (η 10 = 77 mV) and good GOR activity. Density functional theory (DFT) calculations indicate that V and Ru tune the electronic structure of RuV-Co(OH) 2 , greatly increasing the density of the active sites. Moreover, RuV-Co(OH) 2 assembled glucose-assisted hydrogen evolution cell exhibits a battery voltage of 1.42 V for a current density of 10 mA cm −2 , a significant reduction of 240 mV compared to overall water splitting along with higher-value glucose oxidation products. Furthermore, RuV-Co(OH) 2 exhibits outstanding stability. Scanning electron microscopy (SEM), transmission electron microscopy (TEM) and X-ray photoelectron spectroscopy (XPS) analysis demonstrate that RuV-Co(OH) 2 has superior mechanical stability. This work opens up a new approach to designing novel bifunctional electrocatalysts for energy-saving H 2 production and valuable coproductions.
研究领域:
电化学
·
催化
·
材料科学
·
能源转换与存储
✓ 已验证
DOI
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-14
·
IF 14.7
Zhang Minghao,Sun Chenxi,Chen Guanhong,Kang Yuanhong,Lv Zeheng,Yang Jin,Li Siyang,Lin Pengxiang,Tang Rong,Wen Zhipeng,Li Cheng Chao,Zhao Jinbao,Yang Yang
Rechargeable aqueous zinc-metal batteries, considered as the possible post-lithium-ion battery technology for large-scale energy storage, face severe challenges such as dendrite growth and hydrogen evolution side reaction (HER) on Zn negative electrode. Herein, a three-dimensional Cu-In alloy interface is developed through a facile potential co-replacement route to realize uniform Zn nucleation and HER anticatalytic effect simultaneously. Both theoretical calculations and experimental results demonstrate that this bifunctional Cu-In alloy interface inherits the merits of low Zn-nucleation overpotential and high HER overpotential from individual copper and indium constituents, respectively. Moreover, the dynamical self-reconstruction during cycling leads to an HER-anticatalytic and zincophilic gradient hierarchical structure, enabling highly reversible Zn chemistry with dendrite-free Zn (002) deposition and inhibited HER. Moreover, the improved interface stability featured by negligible pH fluctuations in the diffusion layer and suppressed by-product formation is evidenced by in-situ scanning probe technology, Raman spectroscopy, and electrochemical gas chromatography. Consequently, the lifespan of the CuIn@Zn symmetric cell is extended to more than one year with a voltage hysteresis of 6 mV. Importantly, the CuIn@Zn negative electrode is also successfully coupled with high-loading iodine positive electrode to fabricate Ah-level (1.1 Ah) laminated pouch cell, which exhibits a capacity retention of 67.9% after 1700 cycles.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
DOI
高影响因子
Journal of Materials Chemistry A
·
2018
·Vol. 6
·期 22
·10433-10440
·
IF 9.931
Yiping Hu,Feng Li,Yu Long,Haidong Yang,Lili Gao,Xuefeng Long,Haiguo Hu,Na Xu,Jun Jin,Jiantai Ma
Searching for highly efficient, stable and non-noble metal electrocatalysts for the hydrogen/oxygen evolution reaction (HER/OER) is crucial to renewable-energy conversion systems. Cobalt phosphosulfide (CoPS) is regarded as a promising electrocatalyst for the HER in acid solution. Nonetheless, there are no studies of its HER and OER activity in basic solution. Herein, we engineer a novel and highly efficient water splitting electrocatalyst of ultrafine CoPS nanoparticles (NPs) encapsulated in N, P, and S tri-doped porous carbon (CoPS@NPS-C) through metal–organic frameworks (MOFs) and commercial carbon black (XC-72) as precursors. The abundant and evenly distributed metals of MOFs form ultrafine CoPS NPs, and the rich N organic ligands of MOFs and XC-72 are shaped into the NPS-C to protect CoPS NPs leading to long-term stability in water-splitting applications. Meanwhile, the strong interaction between CoPS and NPS-C in this special structure not only ensures the high activity of the HER in acid solution and the OER in alkaline solution, but also maintains good HER performance in alkaline solution. The results display that the novel structure electrocatalyst of CoPS@NPS-C has great potential in water-splitting applications.
研究领域:
材料科学
·
电化学
·
可再生能源
·
催化
✓ 已验证
产品关联
DOI
高影响因子
Journal of Materials Chemistry A
·
2016
·Vol. 4
·期 40
·15536-15545
·
IF 8.262
Zhen Zhu,Yan Yang,Yue Guan,Juanhong Xue,Lili Cui
Hydrogen evolution reaction (HER) and oxygen reduction reaction (ORR) are vital in renewable energy technologies, such as water splitting and fuel cells. Nevertheless, increasing efforts have been paid to develop non-precious metal catalysts as alternatives to noble metal catalysts for HER and ORR. However, how to rationally design and construct an advantageous catalyst is still challenging. Here, a novel cobalt-embedded in nitrogen-doped graphene aerogel (Co–N–GA) catalyst is firstly rationally designed and synthesized by employing a facile strategy of implementing the confined growth of metal organic frameworks (MOFs) within graphene aerogels (GAs). It is worth noting that the Co–N–GA exhibits hierarchical porosity involving micropores, mesopores and macropores, as well as a high surface area (466.6 m2 g−1). More importantly, benefiting from the synergetic effect of hierarchical porosity, high surface area, N-doped carbon and the inner Co metal, the catalyst Co–N–GA displays extraordinarily superior activity for both HER at various pH values and ORR along with better stability. Especially for HER, the onset overpotential, overpotentials@10, 100 mA cm−2 and Tafel slope on the catalyst Co–N–GA in 0.5 M H2SO4 are 0 mV, 46 mV, 183 mV and 33 mV dec−1, respectively. Most importantly, these values are much lower than those of almost all prepared noble-metal-free HER catalysts, indicating the excellent activity for HER of our as-prepared catalyst Co–N–GA. Herein, our strategy opens a new platform to construct a variety of hierarchically porous GA-based catalysts that serve as superior electrocatalysts in energy storage and conversion technologies.
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
危险品化学品经营许可证（带存储）