Journal of Energy Chemistry
·
2024
·
IF 14
Haotian Duan,Wenyang Li,Lixiu Ran,Fulong Zhu,Tianxiang Li,Ming Miao,Wen-jin Yin,Xin Wang,Yongzhu Fu
The conversion of carbon dioxide to ethylene by electrochemical reduction (CO 2 RR) provides a new strategy for achieving carbon dioxide conversion. However, copper-based catalysts have the disadvantages of unsatisfactory selectivity and low current density, which limit the potential CO 2 RR industrial expansion. Researches have verified that the real reaction sites at the catalyst surface often undergo reconstruction during the reaction, therefore, understanding and utilizing this phenomenon is crucial for improving catalytic performance. In this work, we introduced additional Ag component into Cu@Ag/C tandem catalyst by in-situ electrochemical reconstruction of Cu 2 CO 3 (OH) 2 /AgCl/C precursor. This electro-reduced catalyst exhibits a C 2 H 4 Faradaic efficiency of 50.41% in H-cell, and 58.03% in the flow cell, surpassing the counterparts of pure Cu and Ag, as well as the Cu-Ag homolog with separated interface. Moreover, it also provides a long-term stability of 21 h with the ethylene Faraday efficiency (FE) over 50%. The appropriate amount of Ag dopant into the Cu catalyst changes the electronic structure of Cu surface by the electron transfer from Cu to Ag, which distinctly enhances the binding energy of CO 2 on the catalyst. Meanwhile, in-situ Raman results and theoretical calculation reveal that the introduction of silver increases the number of active sites and improves the coverage of *CO intermediate, thereby accelerating the kinetics of C–C coupling and reducing its energy barrier. The combination of cascade catalytic strategy and in-situ electroreduction interface provides potential applications for future artificial carbon balance.
研究领域:
材料科学
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电化学
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催化反应
✓ 已验证
产品关联
DOI
高影响因子
Journal of Materials Chemistry A
·
2025
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IF 9.5
Chenyang Duan,Hao Zhang,Zhiwei Hu,Zhenya Li,Wenjie Bian,Chao Jing,Jian-Qiang Wang,Linjuan Zhang
Modulating the configurational entropy of materials is an effective strategy to develop efficient and robust electrocatalysts for the oxygen evolution reaction (OER) in clean energy technologies. However, the impact of configurational entropy on catalytic activity has received limited attention. In this study, we systematically investigate a class of alloy catalysts composed of Cr, Mn, Fe, Co, and Ni, as a function of Ni content to modulate the configurational entropy to 1.50R (high-entropy alloy, Ni-HEA), 1.23R (medium-entropy alloy, Ni-MEA), and 0.66R (low-entropy alloy, Ni-LEA), where R is 8.314 J (mol−1 K−1). In situ Raman spectroscopy reveals that increased configurational entropy facilitates the formation of the OER active γ-NiOOH phase on the alloy surface. This transition leads to a significant decrease in the OER overpotentials and Tafel slopes. The optimized Ni-HEA exhibits an overpotential of only 217 mV at 10 mA cm−2, and demonstrates prolonged operational stability for 600 hours under industrial conditions. This work enhances our understanding of the impact of configurational entropy on catalytic activity and offers a novel approach for the rational design of porous high-entropy catalysts with improved OER efficiency.
研究领域:
材料科学
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电化学
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清洁能源技术
✓ 已验证
产品关联
DOI
高影响因子
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
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2017
·Vol. 19
·期 36
·24689-24695
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IF 4.123
Minghai Yao,Peng Wu,Shuang Cheng,Lufeng Yang,Yuanyuan Zhu,Mengkun Wang,Haowei Luo,Bangfen Wang,Daiqi Ye,Meilin Liu
α-V2O5 nanowires with a layered structure have been fabricated through a two-step procedure. When measured as a pseudo-capacitive electrode with a three-electrode configuration in 1 M Na2SO4 aqueous solutions, α-V2O5 exhibits ideal capacitive characteristics with a specific capacitance of ∼238 F g−1 at a high current of 2 A g−1, but poor cycling stability with a continuous drop in the first 2000 cycles before it is maintained. To find possible solutions towards this problem, the energy storage behavior of the α-V2O5 electrode has been carefully investigated. In situ Raman analysis suggests that it is electrolytic hydrated cations [Na(H2O)n]+ rather than anions (SO42−) that are involved in the energy storage process through reversible adsorption/desorption on the surface or intercalation/deintercalation at the interlayer of the (001) planes accompanied by interlayer spacing expansion/contraction. Moreover, the electrochemical quartz crystal microbalance results indicate that, besides a reversible mass change, there is a continuous mass loss that may originate from slow dissolution of V2O5, which should bear the main responsibility for the poor stability (initial dramatic drop). Hence, how to inhibit dissolution, such as by coating or adding additives in the electrolyte, is found to be the key approach to improve the stability of V2O5 based electrodes.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF CHEMICAL EDUCATION
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2025
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IF 2.9
Handong Jiao,Qiang Liu,Shuqiang Jiao
High-temperature molten-salt electrochemistry (MSE) is a branch of chemistry that has applications across various sectors, including the chemical, metallurgical, materials, nuclear, and even deep space exploration industries. Consequently, it is significant for chemistry undergraduates to engage in experimental training focused on high-temperature MSE. In this study, we developed an instrument for in situ Raman spectroscopic analysis of electrode processes in molten salts. Utilizing this instrument, we designed a rigorous and feasible experimental scheme, along with a comprehensive evaluation method. The integration of in situ Raman spectroscopy and our experimental protocol enables students to gain profound insights into molten-salt electrode processes while deepening their understanding of the underlying reaction mechanisms. Notably, this pedagogical approach not only cultivates students’ interest in chemistry but also enhances their scientific reasoning skills and exposes them to cutting-edge knowledge.
研究领域:
化学教育
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物理化学
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材料科学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Lixiong Xu,Yifan Yang,Chenyue Li,Rongqian Ning,Jun Ma,Mengqin Yao,Shuo Geng,Fei Liu
The electrocatalytic glycerol oxidation reaction (GOR) is an efficient way to reduce the overpotential of the anodic reaction of electrocatalytic water splitting with abundant high-value byproducts. However, it has always been difficult to reveal a clear reaction path and real active site during the electrocatalytic glycerol oxidation reaction (GOR) process. In this work, NiOOH/Ni 3 S 2 /NF, a model catalyst was synthesized by the two-step method, and the reaction path of the electrocatalytic oxidation of glycerol on NiOOH/Ni 3 S 2 /NF was clearly unveiled by the in situ infrared and Raman analysis. In addition, the TEM after GOR and in-situ Raman intuitively demonstrated that the NiOOH was the real active site during the GOR process. Consequently, the synthesized NiOOH/Ni 3 S 2 /NF catalyst achieved a current density of 10 mA cm −2 at 1.227 V vs . RHE and obtained a high formic acid Faraday efficiency of 97.7 % at a low potential of 1.4 V vs . RHE. This work demonstrates an effective method for unveiling the GOR mechanism and the other relevant electrocatalytic reaction processes.
研究领域:
电化学
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催化科学
✓ 已验证
产品关联
DOI
高影响因子
LANGMUIR
·
2024
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IF 3.7
Hongyu Liang,Xiaojie Xia,Manqiang Liu,Shijing Zou,Tianqiang Yin,Hongfei Li,Yanhu Zhang,Chunying Min,Yongfeng Bu
High load-bearing capacity is one of the crucial indicators for liquid superlubricants to move toward practicality. However, some of the current emerging systems not only have low contact pressures but also are highly susceptible to further degradation due to water adsorption and even superlubricity failure. Herein, a novel choline chloride-based ionic liquid analogues (ILAs) of a superlubricant with triethanolamine (TEOA) as the H-bond donor is reported for the first time; it obtains an ultralow coefficient of friction (0.005) and high load-bearing capacity (360 MPa, more than 2 times that of similar systems) due to adsorption of a small amount of water (<5 wt %) from the air. In situ Raman combined with 1H NMR and FTIR techniques reveals that adsorbed water competes with the hydroxyl group of TEOA for coordination with Cl–, leading to the conversion of some strong H-bonds to weak H-bonds in ILAs; the localized strong H-bonds and weak H-bonds endow the ILAs with high load-bearing capacity and the formation of ultralow shear-resistance sliding interfaces, respectively, under the shear motion. This study proposes a strategy to modulate the interactions between liquid species using adsorbed water from air as a competing ligand, which provides new insights into the design of ILA-based macroscopic liquid superlubricants with a high load-bearing capacity.
研究领域:
材料科学
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摩擦学
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化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Materials Chemistry A
·
2023
·Vol. 11
·期 29
·15717-15723
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IF 11.9
Jia-Wei Zhao,Kaihang Yue,Zi-Xiao Shi,Shu-Yin Wei,Wei-Qian Liang,Gao-Ren Li
In situ spectroscopic characterization has been considered as a key method to study catalytic mechanisms. However, most in situ spectroscopic characterizations can only be used to obtain the overall structure of the catalyst, and its spectral intensity depends on the average information about the catalyst as a whole or in a single area, which makes it difficult to determine the real active site of the catalyst. Herein, to overcome the limitations of traditional in situ spectroscopic characterizations, we developed in situ Raman mapping technology to achieve accurate characterizations of active sites during the oxygen evolution reaction (OER), and this work can directly identify and visualize the real active sites of Ni–Fe catalysts for the OER. The in situ Raman mapping technology clearly shows the surface reconstruction process and dynamic active site of the Ni–Fe catalyst during the OER, namely, Ni is converted to NiOOH and the formed NiOOH/Fe–NiOOH as an active site catalyzes the OER. The visualization of the dynamic active site developed in this paper will promote the understanding of the OER catalytic process and can be used in other homo/heterogeneous catalysis fields.
研究领域:
催化化学
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材料科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
ENERGY & FUELS
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2024
·
IF 5.2
Zhuo-Yi Huang,Chun-Gang Xu,Xiao-Sen Li,Yun-Hao Li,Yi Wang,Zhao-Yang Chen
Hydrate-based carbon dioxide (CO2) sequestration in the deep sea or marine strata is an important process in achieving carbon emission reduction. However, the micro mechanism of gas hydrate formation in a seawater system has not yet reached consensus, which restricts the development of the hydrate-based CO2 sequestration. The basic process of water conversion into hydrates is the transformation from disordered water molecules to a structurally ordered state under specific conditions. The influence mechanism of CO2 hydrate formation in seawater in the presence of solid promoters with or without chemical functional group modification was systematically investigated by combining in situ Raman analysis with macroscopic experiments. The results indicate that the hydrate formation is determined by the transformation from weak hydrogen bonds to strong hydrogen bonds; hydroxyl groups help improve the promoting effect, and the acidity of the solution increases due to the retention of CO2 in the solution, which inhibits the secondary formation of CO2 hydrates.
研究领域:
环境科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
MethodsX
·
2019
·
IF 0
Chengyuan Liu,Zhiwei Liu,Hongkun Niu,Cong Wang,Zhaowen Wang,Bingliang Gao,Jingjing Liu,Mark Taylor
We provide a method for preparation of binder-free cathode for rechargeable aluminum-ion batteries (AIBs). Ultrasonicated natural graphite (u-NG) flakes in N-methylpyrrolidone (NMP) is drop-casted to a carbon fiber cloth (CFC) to obtain binder-free u-GF@CFC cathode for AIBs. We also provide an in-situ Raman spectral technology and the corresponding in-situ Raman cell to determine the mechanism of intercalation/deintercalation reactions of the chloroaluminate ions at cathode of AIBs. The in-situ Raman spectra are recorded using a Raman spectrometer combined with a potentiostat/galvanostat model electrochemical workstation. • A simple preparation method of a binder-free u-GF@CFC cathode is suggested. • The u-GF@CFC cathode is obtained by drop-casting ultrasonicated graphite flakes on the surface and internal gaps of the carbon fiber cloth. • The method includes the in-situ Raman spectral technology and the corresponding in-situ Raman cell.
研究领域:
电化学
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能源材料
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纳米材料
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电池技术
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原位表征
✓ 已验证
DOI
JOURNAL OF RARE EARTHS
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2025
·
IF 7.2
Bolin Zhao,Rana Muhammad Irfan,Chuhao Liu,Shamraiz Hussain Talib,Azhar Mahmood,Li Niu
Rare-earth based transition metal oxides have proved to be the most promising candidates in the exploration of non-precious oxygen evolution reaction (OER) catalysts. However, the knowledge regarding their active sites and electrocatalytic mechanism is very limited due to their different crystallization behaviors and there are still big challenges in the efficient coupling of transition and rare-earth metals with full utilization of active sites. To improve and stabilize OER catalysis, we developed the core-shell CeO 2 @CoNiO 2 nanoplates (NPLs) for enhanced and stable OER catalysis. Surprisingly, CeO 2 shell regulates the electronic structure of CoNiO 2 core and increases the number of active sites and oxygen vacancies to achieve high electrochemical performance in a three-electrode system. Compared with CoNiO 2 nanoparticles, the developed core-shell NPLs exhibit favorable performance with an overpotential of only 206 mV at 10 mA/cm 2 and robust electrochemical stability of 500 h at 10 mA/cm 2 and 300 h at 50 mA/cm 2 . In situ Raman spectroscopy unveils that CeO 2 @CoNiO 2 is structurally more stable than CoNiO 2 , which is consistent with its performance persistence. Besides, theoretical calculations confirm that the Ce shell serves as the active centers for OER, and the formed core-shell metal oxides NPLs promote the adsorption and dissociation of water, thus causing the fast generation of O 2 . This work provides a new perspective for designing highly active core-shell structure of mixed metal oxides of transition and rare-earth metals for OER.
研究领域:
电化学
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材料科学
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催化
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纳米技术
·
能量转换
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Pengyan Wang,Chengmei Ding,Zubing Huang,Jiwei Lv,Meiyan Li,Shiwei Zhang,Xupo Liu,Shichun Mu
For a single-substance catalyst, due to the different adsorption/desorption kinetics of metallic (cationic) and nonmetallic (anionic) sites, it typically catalyzes hydrogen evolution in a single-active-site manner, which greatly limits the activity of catalysts. Thus, herein, we simultaneously activate the anion (P) and cation (Ni) sites in nickel phosphide (Ni2P) and generate highly active P(Ni) dual sites through the substrate effect of NiS2–NiS heterogeneous structures. Theoretical calculation results combined with in situ Raman spectroscopy unveil that the NiS2–NiS substrate effectively regulates the charge distribution to concentrate around the P atom, therefore resulting in Ni and P synergistic dual active sites for water adsorption, water dissociation, and H* adsorption. Accordingly, the dual active site formed enables the Ni2P/NiS2–NiS electrocatalyst to only require an overpotential of 75 mV to achieve a current density of 10 mA cm–2 in alkaline media, very close to the Pt-group noble metal catalyst. This work highlights the critical regulatory role of substrates in activating the anion–cation dual active site in the single metal/intermetallic compound (such as metal phosphides, sulfides, nitrides, carbides, borides, and silicides) that promotes catalytic performance.
研究领域:
材料化学
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电催化
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能源科学
·
纳米材料
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物理化学
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表面科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
·
IF 19.503
Ying Li,Yanyan Wu,Hongru Hao,Mengke Yuan,Zhe Lv,Lingling Xu,Bo Wei
Oxygen evolution reaction (OER) is a key step for electrochemical water splitting and understanding the surface reconstruction of OER pre-catalysts is of vital importance. Herein, hybrid Ni 5 P 4 @FeP nanosheet arrays were evaluated as promising OER pre-catalysts. The dynamic surface evolution was probed by in situ Raman spectroscopy, which revealed that Ni 5 P 4 @FeP was rapidly reconstructed to NiFe 2 O 4 during the anodic scan. The structural instability of amorphous NiFe 2 O 4 led to partial reconstitution to Ni/FeOOH at high oxidation potentials. As-formed Ni/FeOOH@NiFe 2 O 4 hybrid with high structural reversibility was established as a truly active species, which exhibited excellent alkaline OER performance with a low overpotential of 205 and 242 mV under current densities of 10 and 100 mA cm −2 , respectively. This work provides a facile strategy to in situ construct an amorphous spinel/oxyhydroxide hybrid structure using electrochemical activation that holds strong promise for potential application in electrochemical water splitting and related energy devices.
研究领域:
电化学
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材料科学
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催化
✓ 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）