Sustainable Energy & Fuels
·
2020
·Vol. 4
·期 9
·4637-4643
·
IF 5.503
Chun Hu,Wei Zhao,Fuqiang Huang,Jiacheng Wang
Highly active and stable electrocatalysts that can work well in alkaline media are essential for industrial water electrolysis. Herein, we have reported the growth of P and Co co-doped Ru hybrids (RuCo–P) on carbon cloth (CC) through a hydrothermal treatment and the following phosphorization. The modification of Ru by Co and P doping can tune the electronic structure for efficient water dissociation and hydrogen desorption in alkaline solution. The resulting RuCo–P/CC achieves a record low overpotential of ∼4 mV to reach a current density of 10 mA cm−2 for the hydrogen evolution reaction (HER) in 1 M KOH solution, and also shows a small Tafel slope (43 mV dec−1) and outstanding long-term stability. The activity of RuCo–P/CC is significantly superior to that of the commercial Pt/C benchmark and other carbon cloth-supported transition metal-based catalysts. The remarkable alkaline HER performance of RuCo–P/CC could be attributed to the synergistic doping of both Co and P that can effectively reduce the water dissociation barrier and optimize the hydrogen adsorption free energy, respectively.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Shen Zhang,Yuan Rui,Xing Zhang,Rongjia Sa,Feng Zhou,Ruihu Wang,Xiaoju Li
The exploration of the inexpensive and efficient substitutes for platinum-based electrocatalysts is of great challenges for hydrogen evolution reaction (HER). Here, we presented a facile method to achieve highly active, cost-effective and stable HER catalysts, which are composed of ultrafine Co-Ru alloy nanoparticles embedded in heteroatom-free graphitic carbon (Co 1-x Ru x /GC). The optimum catalyst with ruthenium content of 0.93 wt% exhibits remarkable HER activity and the excellent durability, low overpotentials of 14, 39 and 44 mV at −10 mA cm −2 are achieved in alkaline, neutral and acidic media, respectively, which can compete with those in commercial 20 wt% Pt/C and majority of the reported platinum-free catalysts. It has been validated that the confinement effect of SBA-15 induces the formation of ultrafine alloy nanoparticles for generating more active sites. The theoretical simulations reveal that Co-Ru alloy regulates hydrogen adsorption energy to the optimum level, thus resulting in high HER activity. This work provides new methods for the fabrication of ultrafine alloy nanoparticles for the electrocatalysis and other application.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
ACS Applied Nano Materials
·
2024
·
IF 5.3
Hanjun Zou,Yan Tong,Yajie Feng,Yongfeng Zhou,Jiaxun Xiao,Lu Xia,Anku Guha,Barbara Polesso,Bin Zhang,Juanli Liu,Kaiwen Wang
Subnanocluster (SNC) cocatalysts are considered to be promising cocatalysts for photocatalytic hydrogen evolution reaction (HER) due to their rich surface-active sites and high atom utilization efficiency. Herein, a reductant-mediated in situ growth of the atomic clusters procedure is developed to synthesize SNC-Cu serving as advanced cocatalysts on TiO2 nanoparticles for HER. The optimized SNC-Cu/TiO2 catalyst, with 1.8 wt % metal mass loading, exhibits a remarkable hydrogen evolution rate of 6832 μmol g–1 h–1, which is ca. 25-fold that of bare TiO2 (273 μmol g–1 h–1 and comparable to that of 1 wt % Pt-modified TiO2 (7754 μmol g–1 h–1). Meanwhile, decent photostability and recyclability are also certified via a 20 h durability test. Comprehensive electron microscopy and spectroscopy characterizations unveil that the outstanding performance of SNC-Cu/TiO2 can be attributed to accelerated charge separation/transfer and suppressed photoinduced electron–hole recombination. Furthermore, in situ X-ray photoelectron spectroscopy and first-principle calculations reveal that the electron-localized SNC-Cu, with its abundant surface sites, facilitates *H adsorption and desorption, thus enhancing the HER activity significantly. This work highlights the promising potential of constructing noble-metal-free SNCs in semiconductors for photocatalytic HER.
研究领域:
材料科学
·
能源科学
·
化学
✓ 已验证
DOI
高影响因子
ACS Catalysis
·
2019
·
IF 12.221
Xueping Qin,Lulu Zhang,Gui-Liang Xu,Shangqian Zhu,Qi Wang,Meng Gu,Xiaoyi Zhang,Chengjun Sun,Perla B. Balbuena,Khalil Amine,Minhua Shao
Improving the reaction kinetics of hydrogen evolution and oxidation reactions (HER/HOR) in alkaline media is critical to promote the development of alkaline fuel cells and electrolyzers. Here, we prepared Pd3Ru alloy nanocatalysts with Ru segregated on the surfaces, forming adatoms and clusters. This structure dramatically lowered the overpotential of Pd toward HER in 1 M KOH by 104 mV at 10 mA cm–2. The HER activity was even higher than that of Pt (6 mV improvement at 10 mA cm–2). Theoretical simulation results revealed that Ru adatoms/clusters on the surface could weaken the hydrogen-binding energy and promote the OH adsorption, consequently lowering the reaction barrier of the rate-determining step in HER. Our findings are of significance for clarifying the role of Ru in bimetallic catalysts and rational design of more active catalysts for HER/HOR.
研究领域:
材料科学
·
催化化学
✓ 已验证
DOI
高影响因子
JOURNAL OF POWER SOURCES
·
2024
·
IF 8.1
You Li,Weiming Chen,Shengkun Jia,Mulan Tang,Yuxin Zhai,Lulu Zhan,Weiyan Chen
For practical rechargeable aqueous zinc-ion batteries, the long-term cycling stability of the zinc anode remains significantly constrained by its low utilization efficiency and the persistent challenge of hydrogen evolution . This study demonstrates the fabrication of ultrathin zinc electrodes with a robust Zn (002) texture while ensuring an adequate supply of zinc metal for use as an anode material . This approach effectively suppresses the tendency of zinc atoms to undergo deposition transformation due to dislocation-induced phenomena. Compared to zinc foils with higher deposition amount, the ultrathin Zn anode exhibits enhanced resistance to dendrite growth and interfacial side reactions. Assembled symmetrical cells based on this ultra-thin Zn anode show a cycle life of 1750 h (1 mAcm −2 , 0.5 mAhcm − 2 ), maintaining stable cycling for over 100h even at a high depth of discharge (DOD) of 46.23%. Additionally, the full cell couple with V 10 O 24 exhibits a high initial capacity of 429.6 mAh g −1 and a capacity retention of 75.8% after 1000 cycles.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
Industrial Chemistry & Materials
·
2023
·
IF 0
Yu Chen,Chang-Long Tan,Jing-Yu Li,Ming-Yu Qi,Zi-Rong Tang,Yi-Jun Xu
Photocatalytic hydrogen (H2) production coupled with selective oxidation of organic compounds into high-value-added organic intermediates has expansive prospects in the utilization and transformation of solar energy, which meets the development requirements of green chemistry. In this work, high-efficiency hole cocatalyst PdS-decorated In2S3 flower-like microspheres are fabricated for the effective visible-light-driven C–N coupling of amines to imines coupled with H2 evolution. Owing to the establishment of the internal electric field, which further boosts the transfer of photoexcited holes to PdS, PdS–In2S3 exhibits distinctly enhanced photocatalytic redox performance, which is 39.8 times higher for H2 and 14.3 times higher for N-benzylidenebenzylamine than that of the blank In2S3, along with high selectivity and stability. Furthermore, the practicability of dehydrogenation coupling of various aromatic amines to the corresponding C–N coupling products on PdS–In2S3 has been demonstrated and a plausible reaction mechanism has been proposed. This work is anticipated to stimulate further interest in establishing an innovative photoredox platform for selective organic synthesis coupled with H2 evolution in a green and sustainable way.
研究领域:
材料科学
·
化学工程
·
环境科学
✓ 已验证
DOI
JOURNAL OF APPLIED ELECTROCHEMISTRY
·
2022
·Vol. 53
·期 4
·847-860
·
IF 2.925
Liu Zuowei,Guo Xueyi,Tian Qinghua,Xu Zhipeng
Abstract The gallium electrowinning process is always accompanied by hydrogen evolution reaction that results in low current efficiency (CE). In this manuscript, cyclic voltammetry and chronoamperometry studies were carried out to investigate the gallium cathode behavior under various conditions and explore the parameter that is beneficial to improve the CE. The CE of the lead and copper cathodes was higher, while gallium deposited on the titanium, SUS316, and SUS304 cathodes was readily separated. Increasing the overpotential and gallium concentration or decreasing the pH within a certain range was all beneficial to improve the CE, while the temperature had no significant effect on the CE. Kinetic studies of gallium electrodeposition were carried out. The gallium electrodeposition process was determined as mixed control and forced convection is expected to further improve the CE. The apparent activation energy and kinetic current from the electrochemical reactions were determined to be 23.335 kJ mol −1 and 47.6 mA, respectively. Graphical abstract
研究领域:
电化学
·
材料科学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Jie Xu,Sini Wang,Chenglong Yang,Tingting Li,Qiangchun Liu,Xiangkai Kong
To design and synthesize materials for alkaline hydrogen evolution is favorable for industrial hydrogen cycle operation. In this study, we present a facile approach to synthesize free-standing ruthenium-beryllium (RuBe) nanosheets, which possess amorphous phase state and associated with holey structures due to the molten method. The two-dimensional RuBe nanosheets exhibit improved activity than pure Ru counterpart and comparable properties to commercial Pt toward hydrogen evolution reaction in both of alkaline and neutral electrolytes. Based on the experiments and density functional theory calculations, it is suggested that the adsorption and dissociation of water molecules on Ru-based catalyst are much enhanced with the assistance of Be modulation, which are essential for the improved hydrogen production capability under alkaline condition. This work broadens the Ru-based catalyst family and may provide new insights for electrocatalyst development.
研究领域:
材料科学
·
电化学
·
催化
✓ 已验证
DOI
高影响因子
Materials Today Chemistry
·
2021
·
IF 8.301
Y. Ji,W. Luo,Y. Liu,Z. He,N. Cheng,Z. Zhang,X. Qi,J. Zhong,L. Ren
The bottleneck of alkaline hydrogen evolution reaction lies in the kinetically sluggish brought from multistep reaction processes involving water adsorption and dissociation, as well as hydrogen adsorption. In this work, we successfully synthesized o-CoSe 2 /c-CoSe 2 heterostructures anchored on MoSe 2 nanosheets to powerfully promote reaction processes. As an electrocatalyst , it exhibits a low overpotential of 112 mV at 10 mA/cm 2 and a Tafel slope of 96.9 mV/dec for an alkaline hydrogen evolution reaction . Moreover, the as-prepared catalyst can behave as both cathode and anode for overall water splitting , which only requires 1.61 V cell voltage at 10 mA/cm 2 . Significantly, the cell voltage can be further reduced to 1.53 V at 10 mA/cm 2 for water electrolysis under the simulated solar irradiation owing to such a semiconductor-based heterostructure that facilitates the separation of photogenerated charges. Here, the improving overall performance of this ternary electrocatalyst is attributed to the multifunctionality and synergistic interaction of different components in this heterogeneous material . The work provides a novel strategy to design active catalysts simultaneously using electric energy and solar energy for effective water splitting.
研究领域:
材料科学
·
能源化学
✓ 已验证
DOI
高影响因子
Inorganic Chemistry Frontiers
·
2020
·Vol. 7
·期 13
·2497-2505
·
IF 5.958
Tong Liu,Changji Fang,Bansui Yu,Yu You,Haihong Niu,Ru Zhou,Junjun Zhang,Jun Xu
Two-dimensional layered MoS2 nanosheets are regarded as a promising catalyst for electrocatalytic hydrogen generation but suffer from limitations of catalytically inert basal planes and poor intrinsic conductivity. In this work, we report a simple hydrothermal method to synthesize defect-rich MoS2 nanosheets featuring vanadium (V) doping, widely expanded interlayer spacings, and a high content of metallic 1T-phase towards the efficient hydrogen evolution reaction (HER). The structural characteristics of V(IV)&V(II) co-doping, mixed 1T&2H phases and wide interlayer expansion endow the nanosheets with plentiful disorders and rich defects, thereby resulting in abundant active sites. Furthermore, V(IV)&V(II) co-doping brings in electronic benefits of a narrowed bandgap, improved intrinsic conductivity and optimized hydrogen adsorption free energy of basal planes. By tuning the V dopant content, the 10%V-MoS2 catalyst shows an optimized HER performance with a low overpotential of 146 mV at 10 mA cm−2 and a small Tafel slope of 48 mV dec−1, and a long operational stability of 80 h. Our work opens up new opportunities for improving the electrochemical HER performance of layered transition metal dichalcogenides (TMDs) by synergistic structural and compositional modulations.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
Nanoscale
·
2020
·Vol. 12
·期 16
·9246-9254
·
IF 6.895
Junxiao Huang,Xuelei Pan,Xiaobin Liao,Mengyu Yan,Bruce Dunn,Wen Luo,Liqiang Mai
1T-MoS2 is widely used in the hydrogen evolution reaction (HER) due to its abundant active sites and good conductivity. However, 1T-MoS2 is thermodynamically metastable due to the distorted crystal structure. Recently, researchers have detected the J1 and A1g Raman peaks after the HER process and confirmed that the 2H–1T phase possesses good stability. Therefore, continuous HER is likely to transform 1T-MoS2 into a stable 2H–1T mixed phase. The in situ characterization of 1T-MoS2 individual nanosheets in the HER process is important to understand the intrinsic electrocatalytic behaviour at confined nanoscale, which has rarely been investigated. Herein, we built an individual 1T-MoS2 nanosheet micro–nano device by the intercalation of N-butyllithium into 2H-MoS2. Then, the device was kept at an overpotential (η) of 450 mV, which was much lower than the onset potential, for 20 minutes to ensure continuous HER. Through this electrochemical treatment, we successfully obtained a mixed phase of 2H–1T and monitored the electrochemical phase transition by in situ Raman mapping and atomic force microscopy (AFM). The HER performance of the 2H–1T phase was superior to that of 1T-MoS2 and 2H-MoS2. Additionally, computational simulations demonstrated that the 2H–1T phase exhibited optimal hydrogen adsorption energy. The presented work displays the excellent catalysis of the mixed phase obtained by the electrochemical phase transition, which provides new directions for improving the catalytic activity of TMDs.
研究领域:
材料科学
·
电化学
·
纳米技术
✓ 已验证
DOI
高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2021
·Vol. 168
·期 11
·114504
·
IF 4.316
Yinling Wang,Nannan Ma,Mingli Fan,Wujian Tang
Transition metal phosphides (TMP) are excellent non-precious metal electrocatalysts for hydrogen evolution reaction (HER). The generation of PO43− before and during the HER process may be inevitable due to the instability of TMP. To investigate the effect of PO43− on the HER catalytic activity of electrocatalysts in alkaline medium, NiCo-S nanotubes were modified with phytate (PHY) with six phosphate groups via adsorption. The successful modification was verified by zeta potential, FT-IR, element mapping, XPS, etc The NiCo-S/PHY displayed a higher HER activity than original NiCo-S. Under the optimum adsorption time (7 h), the overpotential at 10 mA cm−2 (η10) of NiCo-S/PHY (173 mV) was only half that of the original NiCo-S (346 mV). The role of PO43− was discussed in detail. Moreover, this strategy was extended to NiCo-S grown directly on nickel foam (NiCo-S/NF) and the corresponding NiCo-S/PHY/NF also showed superior HER activity and good stability. This work provides a new strategy to improve the HER activity of electrocatalysts and also a novel perspective for the HER mechanism of TMP.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）