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Current Issue
2024 Vol.41 Issue.5,
Published 2024-09-15
Special issue on hydrogen energy
0
2024 Vol. 41 (5): 0-0 [
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Special issue on hydrogen energy
1
Editorial: The future of hydrogen energy: Challenges and opportunities in production, storage, and utilization
LI Xiaopeng, XIAO Qi
2024 Vol. 41 (5): 1-3 [
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4
Research progress of key materials for electrocatalytic valorization of alcohols coupled with hydrogen production
PENG Xuan, WU Xiaotong, HUANG Shixian, TAN Lei, LIN Chao, XIAO Qi, LI Xiaopeng
The electrolysis of water for hydrogen production based on green electricity is of great significance for achieving carbon neutrality. However, the sluggish kinetics of the oxygen evolution reaction (OER) at the anode, which requires a high overpotential, significantly limits the efficiency of water electrolysis for hydrogen production. In the field of green hydrogen production, traditional water electrolysis technologies face challenges such as slow kinetics of the anodic oxidation reaction and high production costs, severely limiting their commercialization. By using organic small molecule oxidation reactions with better thermodynamic and kinetic performance to replace traditional OER, energy consumption can be effectively reduced and energy efficiency improved, meanwhile the generation of value-added small molecule chemicals can also significantly enhance the technical and economic feasibility of this reaction pathway, thereby broadening the market application prospects of green hydrogen production technologies. This review focuses on the widely studied systems of electrocatalytic oxidation reactions of small molecule alcohols and their reaction mechanisms. We systematically summarize the research progress of high-performance anode catalytic materials systems applicable to alcohol small molecule electrolysis for hydrogen production. We also present the remaining challenges in electrocatalytic oxidation reactions of alcohols and prospects for future development directions in this field. The aim is to provide some guidance for the commercial application of anodic oxidation of small organic molecules for replacing OER.
2024 Vol. 41 (5): 4-18 [
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19
Research progress of bipolar membranes and their application in hydrogen energy
YAO Xinyun, QIAN Huidong, ZHAO Hongbin
Renewable energy conversion technologies that utilize hydrogen energy, such as fuel cells and water electrolyzer to produce hydrogen, play a key role in the target of carbon dioxide emission peak and carbon neutrality. Bipolar membrane fuel cells and bipolar membrane water electrolyzer are new electrochemical energy conversion devices that use bipolar membranes as electrolytes and have been proposed in the past decade. Starting from the water dissociation mechanism of bipolar membranes, this article introduces the composition, interfacial layer structure and preparation process of bipolar membranes in detail, and reviews and prospects the applications of bipolar membranes in different fields. Among them, the domestic and abroad research progress of bipolar membranes in the fields of fuel cells and water electrolyzers is mainly introduced, and the unique advantages of application brought by the bipolar membrane structure as well as the key issues and prospects for application are summarized.
2024 Vol. 41 (5): 19-34 [
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92
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35
Cracking causes and new solutions of Ni-Mo coating on hydrogen evolution electrode
ZHOU Weishan, MIN Luofu, CHEN Yanan, ZHANG Wen, XU Li, WANG Yuxin
In the field of hydrogen production by alkaline water electrolysis, electroplated nickel-molybdenum alloy electrodes have attracted much attention because of their high hydrogen evolution activity and simple preparation. However, the widespread cracking and peeling off of the nickel-molybdenum plating seriously affects the performance and stability of the electrode. The aim of this study is to investigate the mechanism of cracking and peeling of nickel-molybdenum electrodes and to propose a new method to avoid the cracking of the plating layer. Through the observation of bubble precipitation, crack monitoring and electrochemical measurements in the plating layer, this paper reveals that the reason of cracking of nickel-molybdenum plating layer is the shrinkage of the plating layer and the internal stress due to the release of hydrogen that enters the plating layer with the electrodeposition of the metal. A new method of nickel-molybdenum electrodeposition with low bath concentration and high current density is then proposed. The new electrodes did not crack and the overpotential was only 260 mV at 400 mA·cm
-2
current density in 1 mol·L
-1
KOH alkaline solution, which was 55 mV lower than that of the nickel-molybdenum coating electrode which are susceptible to cracking. The new method not only solves the cracking and peeling problem of nickel-molybdenum electrodeposition, but also improves its hydrogen precipitation performance.
2024 Vol. 41 (5): 35-42 [
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43
Ruthenium-doped preparation of mixed crystalline phase molybdenum carbide for hydrogen evolution reaction
ZHANG Jiazhu, SUN Yongli, YANG Xiaodong, YANG Na, JIANG Bin, XIAO Xiaoming, TANTAI Xiaowei, ZHANG Lvhong
Ru atoms were uniformly loaded on the surface of self-assembled micrometer spheres of nitrogen-doped ultrathin molybdenum carbide nanosheets by ion-exchange method, and the ratio of
β
-Mo
2
C and
α
-MoC
1-
x
in Ru-Mo
x
C NFs was adjusted by adjusting the content of ruthenium in the precursors, Ru-Mo
x
C NFs-4 catalyst with excellent hydrogen precipitation performance was obtained, which exhibited very good hydrogen precipitation performance due to the better hydrogen adsorption energy of the mixed crystalline phase molybdenum carbide and the synergistic effect between Ru and Mo
2
C substrates. Ru-Mo
x
C NFs-4 exhibited low overpotentials (
η
10
=49 mV and
η
100
=127 mV), a Tafel slope of 51.3 mV·dec
-1
, and good durability. This study provides a new idea for the design of efficient catalysts for hydrogen evolution reaction by tuning the carbide phase composition through doping with metals.
2024 Vol. 41 (5): 43-50 [
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95
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51
Electrodeposited highly active and stable Ni-Fe alloy electrodes towards oxygen evolution reaction
LI Yue, MIN Luofu, ZHANG Wen, XU Li, WANG Yuxin
We prepared porous nickel-iron alloy electrodes for alkaline water electrolysis oxygen evolution reaction (OER) by electrodeposition on a commercial nickel mesh. By regulating the quality of electrodeposition and the concentration of metal ions in the plating solution to change the deposition layer morphology, catalytic performance, and stability of the electrode catalyst, a multi-stage porous dendritic morphology plating was prepared. At a current density of 10 mA·cm
-2
, the electrode OER overpotential was only 250 mV, and the Tafel slope was only 35.8 mV·dec
-1
. The catalytic activity exceeded that of the commercial Ir catalyst, and the
C
dl
value reached 14.43 mF·cm
-2
, which was 10 times that of the blank Ni mesh, providing excellent OER catalytic activity with a large electrochemical active area. Meanwhile, the porous morphology constructed by electrodeposition reduced the reaction resistance, and the
R
ct
value of the NiFe alloy electrode (0.32 Ω) was much smaller than that of the Ir/Ni electrode (1.51 Ω), which possessed faster catalytic reaction kinetics. Under the conditions of 80 ℃, 30% KOH and 500 mA·cm
-2
current density, the stable operation of water electrolysis for 75 h did not show any significant degradation, which demonstrated good stability.
2024 Vol. 41 (5): 51-60 [
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61
A numerical simulation of membrane-less water electrolyzer with flow-through-electrodes
SHEN Cen, LIU Bolun, MIN Luofu, XU Wei, WANG Yuxin
It is an ideal way to produce hydrogen by converting renewable energy into hydrogen energy using hydroelectricity. At conventional electrolysis, membrane occupies a large proportion in the cost of electrolytic device and brings high resistance, and the degradation of membrane is a short board that affects the life of electrolytic system. Membrane-less water electrolysis technology can effectively avoid the cost, life and resistance brought by membrane, which has great research significance. A two-dimensional numerical simulation model of membrane-less electrolysis with flow-through electrode was developed in this study firstly, taking the mass transport, momentum transport, electrochemical reaction, charge transport and their coupling relationship into comprehensive consideration. The ratio of overpotential in the total voltage caused by electrode activation, active area covered by bubbles and ohmic impedance was analyzed, and the influence of electrolyte flow rate and electrode gap thickness on the voltage drop of the whole system was emphatically studied. The results show that the active area covered by bubbles and the overpotential caused by ohmic impedance play a major role in the total voltage, both of which can be reduced by increasing electrolyte flow rate and decreasing electrode gap thickness. In order to ensure the electrolytic efficiency of the system and reduce the gas content in the gap, it is necessary to coordinate the electrolyte flow rate, current density and electrode gap thickness, so as to achieve the optimal performance.
2024 Vol. 41 (5): 61-72 [
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84
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73
Research progress of external field assisted strategies for hydrogen production by water electrolysis
SHI Qiwei, YAN Yifan, LUO Lan, LI Zhenhua
The technology of hydrogen production by water electrolysis holds significant promise for energy storage and conversion. Despite considerable efforts in designing and modifying electrocatalysts to enhance performance, the field has encountered a bottleneck, which prompts the exploration of alternative methods for breakthroughs. A noteworthy approach involves the application of external fields (such as light, magnetic, elastic stress, and gravity fields) to improve mass transfer and alter reaction kinetics. This innovative strategy aims to overcome current challenges and substantially boost electrocatalytic performance. This review focuses on the latest advancements in external field-assisted strategies for hydrogen production from water electrolysis (encompassing the hydrogen evolution reaction, oxygen evolution reaction, and coupled organic oxidation reaction), hoping to contribute to the further development of high-performance hydrogen production technologies.
2024 Vol. 41 (5): 73-85 [
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89
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86
Red phosphorus/carbon nitride heterostructure for photocatalytic overall water splitting
PEI Zeyu, WANG Wancheng, ZHU Yuanzhi
In order to solve the problem of easy recombination of photogenerated carriers and pollution caused by sacrificial agents in the photocatalytic cracking of red phosphorus materials, a heterostructure of crystalline red phosphorus and carbon nitride (M-CN/C-RP) was designed and constructed. The results show that this heterostructure can significantly improve the efficiency of hydrogen production by photocatalytic cracking of water, and avoid the effect of sacrificial agents on the results of photocatalytic hydrogen production. Without the addition of sacrificial agent, the photocatalytic hydrogen production rate of M-CN/C-RP with heterostructure can reach 30.7 μmol·h
-1
, and it has better stability and can produce hydrogen continuously within 20 h.
2024 Vol. 41 (5): 86-92 [
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85
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93
Research progress of organic semiconductor photocatalysis for hydrogen evolution reaction
WANG Siyue, HAN Bing, SHAO Yang, JIA Yihui, WANG Boya, ZHU Xiaolin
Utilizing semiconductor materials for solar-driven hydrogen production is an alternative to hydrogen generation using fossil fuels. Organic photocatalysts, composed of abundant elements such as C, H, and O on Earth, have the advantage over inorganic catalysts due to their tunable electronic properties through molecular engineering. However, the current understanding of the key properties of their photocatalytic oxidation-reduction process is not complete, hindering further development into more cost-effective and competitive technologies. This paper reviews the progress in organic semiconductor photocatalysis and research on its mechanisms. Starting with the description of charge transfer in organic semiconductors, it outlines the current state of research on the hydrogen evolution reaction (HER) of organic photocatalysts, analyzes the behavior of excitons after photoexcitation, and proposes strategies to improve the efficiency of hydrogen production by organic semiconductor photocatalysis. Finally, it summarizes the research progress on conjugated supramolecular and the development of organic photocatalyst is expected and prospected.
2024 Vol. 41 (5): 93-113 [
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105
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114
Optimal pressure configuration of 70 MPa cascade hydrogen refueling station based on least squares method
ZHONG Yongbin, WU Xuan, OUYANG Yanchao, ZHU Qiao, YANG Jin
The optimal pressure configuration of the 70 MPa cascade hydrogen refueling station is quickly and accurately solved by using the least squares method (LSM), and the optimal pressure levels of each hydrogen storage tank are obtained. Firstly, the mathematical models of hydrogen state, on-board hydrogen cylinder, hydrogen dispenser and compressor are established under cascade hydrogen refueling system, and compared with the experimental data at 5.5 MPa initial pressure and 298 K ambient temperature, the correctness of the models is verified. Secondly, the energy consumption model of the hydrogen filling process is established, and the pressure configuration is converted into the optimization of pressure ratio. The optimal pressure ratio formula is obtained based on the LSM. Finally, using LSM, for the cascade hydrogen refueling station whose hydrogen source is 20 MPa hydrogen tube trailer, the optimal pressure of the three-stage hydrogen refueling station is 30, 57 and 88 MPa, respectively. Compared with the traditional sequential search method, the total energy consumption is reduced by about 2.4%. The energy efficiency of cascade hydrogen refueling is improved by 36% compared to traditional single-stage hydrogen refueling stations.
2024 Vol. 41 (5): 114-120 [
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121
Enhancement of In
2
O
3
catalytic performance for CO
2
hydrogenation to methanol by regulating Ni doping
LI Pingping, GUAN Linjie, ZHANG Long, DING Maofeng, XU Danyun, XIE Delong
The development of indium-based catalysts with high activity and stability for promoting carbon dioxide hydrogenation to methanol is indeed a significance area of research for advancing green and sustainable technologies. The introduction of Ni into indium oxide through the co-precipitation method has been shown to effectively modulate the structure and surface properties of the crystal, leading to enhanced catalytic performance. In results, it was found that at a Ni content of 2.5%, Ni primarily exists as highly dispersed Ni
2+
within the crystal structure, which significantly increases the oxygen vacancy content on the surface of the material. While at a higher Ni content of 10.0%, Ni exists not only in the form of Ni
2+
, but also partly in the metallic form. Comparing the catalytic performance of indium oxide with different nickel content at 260 ℃, 3 MPa and space velocity of 8 000 mL·g
-1
·h
-1
, 2.5% Ni@In
2
O
3
exhibits better catalytic performance, achieving CO
2
conversion of 5.5% and methanol selectivity of 36.5%. This suggests that controlling the Ni content and its chemical state in indium oxide catalysts can optimize the oxygen vacancy on the surface of In
2
O
3
and enhance the activity of catalyst.
2024 Vol. 41 (5): 121-130 [
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131
Pd supported on FeS
2
-rGO composite carrier for efficient selective hydrogenation of nitroarenes
WANG Rui, TAN Xiaojie, LI Xudong, LIU Yachao, LIU Tengfei, CUI Shihao, ZHAO Qingshan
Palladium-based catalysts are known as effective catalysts for hydrogenation reactions with wide applicability, while the excessive hydrogenation activity limits their application in selective hydrogenation reactions. In this study, a novel Pd/FeS
2
-rGO catalyst was prepared by loading palladium onto a FeS
2
-rGO composite carrier, and its catalytic performance towards the selective hydrogenation of nitroarenes to aromatic amines was investigated. The Pd/FeS
2
-rGO catalyst was characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), and X-ray photoelectron spectroscopy (XPS). The influence of the carrier on the catalytic performance was explored. The results show that the FeS
2
-rGO composite carrier can well disperse and regulate the electron density of Pd, resulting in a 99% conversion and selectivity for the hydrogenation of 4-chloronitrobenzene over the Pd/FeS
2
-rGO catalyst. In addition, the catalyst also showed excellent universality and cycling stability for the selective hydrogenation of various nitroarenes, which could be recycled six times without performance degradation. This study provides a new idea for developing high-efficiency catalysts for the selective hydrogenation of nitroarenes.
2024 Vol. 41 (5): 131-140 [
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89
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179
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141
Effect of hydrochar-modification on catalytic performances of Pt catalysts in selective hydrogenation phenol and furfural
ZHANG Wenwei, ZHOU Wei, MA Xueqin, LAI Haichen, ZHANG Xingguang
Supported Pt catalysts play a significant role in the selective hydrogenation of bio-derived chemicals. In this study, the typical MAX phase of Ti
3
AlC
2
was used as the precursor to prepare Pt catalysts in one pot. Introduction of glucose as the hydrochar resource, a series of hydrochar-modified Pt catalysts were developed with different hydrochar contents. Characterizations of XRD, TEM, SEM, XPS and ICP were employed to analyze catalysts crystal phases, Pt particle size and distribution, morphologies, chemicals states of key elements and Pt real content. These catalysts were evaluated in the selective hydrogenation of bio-derived model chemicals such as phenol and furfural to investigate catalytic performances. The results demonstrated that the hydrochar-modified catalysts of Pt/Ti
3
Al
x
C
2
T
y
-glucose improved catalytic activity, selectivity, or stability, as compared with Pt/Ti
3
Al
x
C
2
T
y
. The possible reasons are due to the adsorption effect of hydrochar surface functional oxygen-containing groups, which enrich reactants and boost reaction kinetics, meanwhile, the hydrochar stabilizes Pt NPs by reducing aggregation to enhance stability.
2024 Vol. 41 (5): 141-153 [
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90
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183
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154
Study on hydrogenation of fatty acid methyl ester catalyzed by Cu-Zn-Al catalyst
JIANG Feng, XU Yunqiang, XU Yan, ZHAO Yujun
The effect of copper loading and Cu-Zn ratio on the hydrogenation of methyl laurate to fatty alcohol over Cu-Zn-Al catalyst was studied. The results show that Cu-Zn-Al catalyst has excellent hydrogenation activity of fatty acid methyl ester. Under the conditions of 5 MPa, 190 ℃ and 2 h
-1
, the conversion of fatty acid ester and selectivity of fatty alcohol are up to 78.87% and 89.14%, respectively, which are much higher than Cu/Al
2
O
3
and Cu/ZnO catalysts. The reason is that the Cu-O-Zn site generated by the interaction between zinc species and copper species improves the catalytic activity of Cu
0
, with a high TOF value (27.5 h
-1
). Aluminum species as a structural promoter improve the specific surface area and enhances the stability of the catalyst. When the temperature is increased to 210 ℃, the conversion of methyl laurate and the selectivity of lauryl alcohol can be up to 99%, showing high catalytic performance and application value.
2024 Vol. 41 (5): 154-163 [
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102
) [
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205
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164
Advances of supported nano-catalysts for selective semi-hydrogenation of alkynes
LI Yaying, XUE Chen, JIA Weijie, LI Xiaopeng, XIAO Qi
Alkenes represent a crucial category of organic compounds, extensively utilized in the synthesis of pharmaceuticals, pesticides, and polymers. The selective semi-hydrogenation reaction serves as an effective method to transform alkynes into alkenes, bearing significant practical production value. In recent years, supported nano-catalysts have exhibited notable advantages in the domain of selective semi-hydrogenation of alkynes. This review provides a comprehensive overview of the advancements in the use of supported nano-catalysts for the selective semi-hydrogenation of alkynes over the past five years. It briefly introduces the mechanism of the alkyne semi-hydrogenation reaction, and discusses the factors influencing the enhancement of reaction selectivity by these nano-catalysts. Furthermore, it summarizes the research progress concerning typical supported nano-catalysts in thermocatalytic, electrocatalytic, and photocatalytic selective semi-hydrogenation of alkynes. Finally, it offers a forward-looking perspective on the future potential of supported nano-catalysts in alkyne semi-hydrogenation reactions.
2024 Vol. 41 (5): 164-182 [
Abstract
] (
110
) [
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1KB] [
PDF
4957KB] (
197
)
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