GREEN CHEMISTRY
·
2025
·
IF 9.2
ZhiWei Dong,YaLing Jia,Zeyu Wang,Antony Rajendran,Wen-Ying Li
Electrocatalytic CO2 reduction to formic acid is a promising strategy to obtain value-added chemicals and achieve the carbon cycle. However, its practical application is generally impeded by the limited accessibility of CO2 to the catalyst's surface and the lack of efficient universal catalyst across different pH levels. Herein, we report a new catalyst, i.e., SnS2 decorated with hydrophobic polymer polyvinylidene fluoride (SnS2+PVDF), for the effective electrocatalytic CO2 reduction to formate/formic acid across a wide pH range in a flow cell. This catalytic system accomplishes a remarkable Faradaic efficiency for the formic acid production in alkaline (98%), neutral (86%), and acidic (93%) electrolytes. Also, the single-pass carbon efficiency reaches up to 72.77% in acidic electrolyte. Water contact angle measurements in association with the in-situ attenuated total reflectance surface-enhanced infrared absorption spectroscopy results indicate that the inclusion of PVDF creates a hydrophobic microenvironment which increases the CO2/H2O ratio near the surface of SnS2 particles. As a consequence, SnS2 particles enjoy the enhanced CO2 concentration around their surface to form many three-phase (solid-liquid-gas) boundary. In-situ Raman spectra combined with electrocatalytic studies reveal that SnS2 undergoes reconstitution to form catalytically active Sn/SnS2 during the reaction. These findings ensure and expand the generality of hydrophobic microenvironment regulation strategy in promoting electrocatalytic CO2 reduction to formic acid.
研究领域:
化学
·
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
Nanoscale
·
2024
·Vol. 16
·期 23
·11250-11261
·
IF 5.8
Tingxia Wang,Xu Zhang,Xiaojiao Yu,Yun Liu,Junpeng Li,Zongbin Liu,Ningning Zhao,Jian Zhang,Jinfen Niu,Qingliang Feng
High-efficiency water electrolysis over a broad pH range is desirable but challenging. Herein, Ru-decorated VS2 on carbon cloth (Ru–VS2/CC) has been in situ synthesized, which features the regulated electronic structure of VS2 by introducing Ru. It is remarkable that the optimal Ru–VS2/CC displays excellent electrocatalytic hydrogen evolution activity with overpotentials of 89 and 87 mV at −10 mA cm−2 in 0.5 M H2SO4 and 1.0 M KOH, respectively. Theoretical calculations and electrocatalytic measurements have demonstrated that introducing Ru induces an enhanced charge density around the Fermi level, facilitating charge transfer and speeding up the electrocatalytic HER kinetics. The Gibbs free energy of the hydrogen intermediate (ΔGH*) of Ru–VS2/CC (0.23 eV) is much closer to zero than that of pure VS2 (0.51 eV) and Ru (−0.37 eV), demonstrating an easier hydrogen adsorption and desorption process for Ru–VS2/CC. The more favorable ΔGH*, differential charge density and the d-band center endow Ru–VS2 with enhanced intrinsic electrocatalytic activity. This study presents a feasible strategy for enhancing electrocatalytic HER activity by the regulation of the electronic structure and the rational integration of dual active components.
研究领域:
材料科学
·
电催化
·
理论计算
✓ 已验证
产品关联
DOI
PubMed
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2024
·
IF 8.1
Xiaojing Dong,Yangyang Wang,Jintao Wang,Yiqiang Sun,Bo Xu,Cuncheng Li,Lifeng Hang
In the field of research on renewable energy conversion and storage methods, the development of catalysts with excellent properties and outstanding stability for oxygen evolution reaction (OER) acting at various pH values has become a much-anticipated research focus. RuO 2 as a benchmark OER catalyst, its wide application has always been limited by slow reaction kinetics and limited persistence. In this paper, Mn-doped RuO 2 material was developed and the optimum doping ratio was identified for using as an OER electrocatalyst under general purpose pH media. Mn 0.1 Ru 0.9 O 2 exhibited a lower overpotential value of 224 mV in acidic environment with a Tafel slope value of 51.62 mV dec −1 . Moreover, in alkaline and neutral environments, overpotentials of 231 mV and 376 mV were required to obtain a current density of 10 mA cm −2 , respectively. In addition, through continuous stability testing over 24 h in alkaline, acidic and neutral solutions, it has been further demonstrated that the Mn-doped RuO 2 material exhibits extremely high stability. The advancements in this research offer crucial insight into the rational development of efficient and durable RuO 2 -based catalysts.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Catalysis
·
2021
·
IF 13.084
Jiayi Qin,Cong Xi,Rui Zhang,Tao Liu,Peichao Zou,Deyao Wu,Qianjin Guo,Jing Mao,Huolin Xin,Jing Yang
It is highly desirable to develop all-pH-compatible hydrogen evolution reaction (HER) electrocatalysts that can be used universally in a variety of different electrolyzers and operated in different pH conditions, i.e., acid, alkaline, microbial, chlor-alkali, etc. So far, two-dimensional layered MoS2 and Mo-based carbon materials have been regarded as promising pH-universal HER electrocatalysts. 2H-MoS2 as a naturally occurring and thermodynamically favorable phase, yet still suffers from poor HER activity in neutral and alkaline electrolytes. Herein, a hybrid electrocatalyst, i.e., 2H-MoS2/N-doped mesoporous graphene, rich in interfacial Mo–pyridinic N coordination is fabricated. The optimized hybrid catalyst delivers long-term durability and outstanding HER activity with overpotentials of 110, 145, and 142 mV at 10 mA cm–2 in acidic, alkaline, and phosphate buffered solutions (PBS) media, respectively, outperforming most of the previously reported MoS2-based catalysts. Theoretical and experimental results demonstrate that the interfacial pyridinic N has a higher tendency to bond with Mo atoms than pyrrolic and graphitic N, and the edge-Mo coordinated with pyridinic N could serve as HER active sites. DFT calculations further reveal that Mo–pyridinic N coordination modifies the charge density of edge-Mo, in turn optimizing the hydrogen absorption energy and facilitating water dissociation, and thereby significantly promoting the intrinsic catalytic activity for the pH-universal HER process.
研究领域:
材料科学
·
电化学
·
催化科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Jiachen Li,Cong Zhang,Chi Zhang,Huijun Ma,Yong Yang,Zhaoqi Guo,Yaoyu Wang,Haixia Ma
Replacing sluggish oxygen evolution reaction (OER) by hydrazine oxidation reaction (HzOR) is an energy-saving approach to assist alkaline overall water splitting (OWS). However, it is still at the infant stage as the unsatisfactory of the design strategies for bifunctional catalysts toward both HzOR and hydrogen evolution, which leads to high working potential compared to the theoretical value. Here, for the first time, we report a galvanostatic immobilization of ruthenium single atoms (Ru SAs) into the oxygen vacancy of urchin-like tungsten trioxide (Vo-WO 3 ) and show low overpotentials of 17, 34, and 64 mV at –10 mA cm –2 under acid, alkaline, and neutral H 2 evolution, respectively. As an efficient bifunctional catalyst, the Vo-WO 3 /Ru SAs is firstly introduced to HzOR and achieves low working potential of –58 mV at 10 mA cm –2 . The HzOR-assisted OWS also delivers an ultralow cell voltage of only 25 mV at 10 mA cm –2 in alkaline medium, which is far beyond the platinum and most of the state-of-the-art catalysts. Additionally, this coupled system can also be well performed under neutral condition, realizing a cell voltage of only 137 mV at 10 mA cm –2 . The excellent pH-universal HzOR-assisted OWS activity is attributed to the particular electronic configuration between Ru SAs and WO 3 , the immobilization of Ru SAs in WO 3 could induce electron redistribution and optimize free energy of hydrogen adsorption in hydrogen evolution, while the isolation of Ru SAs also leads to the electropositivity of W sites and tends to accelerate the oxidation of hydrazine.
研究领域:
材料科学
·
催化化学
·
能源科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2020
·
IF 7.632
Ying Zheng,Yangdong Chen,Xin Yue,Shaoming Huang
Tuning electronic structures through heteroatom doping to weaken the Mo–H binding strength and constructing larger specific surface areas are considered an effective strategy to improve the hydrogen evolution reaction (HER) activity on β-Mo2C in full pH range. In this report, a CH4 (10%)/H2 inducing universal method for the formation of heteroatom-doped (F, N, S, or B) β-Mo2C nanoparticles (NPs) with nanosized and clean surface supported on reduced graphene oxide (rGO) (Mo2ExC1–x/rGO, E = F, N, S, or B) is proposed. Doping with different heteroatoms introduced different promoting effects on Mo2C toward HER in the full pH range. The Mo2FxC1–x/rGO electrocatalysts show the best activity for HER in acidic, alkaline, and neutral media, with the onset overpotentials of 37, 45, and 105 mV, respectively, which achieve 10 mA cm–2 at overpotentials of only 95 mV in 1 M HClO4. More noteworthy is the fact that the Mo2FxC1–x/rGO electrocatalysts only require 232 and 397 mV of overpotentials to reach 400 mA cm–2 in acidic and alkaline solutions, respectively. Besides, the Mo2FxC1–x/rGO electrocatalysts only need 480 mV of overpotential to reach 200 mA cm–2 in neutral conditions. Meanwhile, larger specific surface areas with nanosized and clean surfaces also contribute to improving the performance of HER, especially Mo2FxC1–x/rGO. However, the promoting effect of HER by tuning the electronic structures through doping of B and S into Mo2C is very limited. Moreover, doped Mo2C-based electrocatalysts in this work show superior stabilities for HER in the full pH range.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Jiaxin Yuan,Jianrui Feng,Gang Li,Yinghao Song,Na Yu,Xi Chen,Guanjie He,Yeshu Tan,Meng Ni
Developing efficient electrocatalysts for pH-universal hydrogen evolution reaction (HER) is particularly appealing due to the growing demands of clean and renewable energy. Herein, a facile electrodeposition method to construct Rh nanoclusters supported by molybdenum trioxide micro sheets (Rh/MoO 3 ) was developed. The use of MoO 3 support can enhance hydrogen production due to the accelerated electron transfer by Mo. The interaction between the interface of Rh and MoO 3 modulates the hydrogen adsorption energies. The interfacial electron transfer from Rh to Mo optimizes H 2 O adsorption, adjusts the d-band center, and fine-tunes the hydrogen binding energy, hence increasing the inherent hydrogen-evolving activities. Therefore, the Rh/MoO 3 catalyst shows outstanding performance with very low overpotentials of only 34, 49, and 29 mV at a current density of −10 mA cm −2 in 1.0 M PBS, 0.5 M H 2 SO 4 , and 1.0 M KOH electrolytes, respectively. Our findings also help to create effective catalysts for pH-universal HER by leveraging particle-support interactions.
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
iScience
·
2024
·
IF 4.6
Meng Wang,Xiaoyu Li,Yanrui Su,Jiaoge Wu,Tian Sun,Xuan Xu,Faying Fan,Yufei Zhao,Wa Gao
Fenton or Fenton-like reactions have been widely used in various fields, including solar energy conversion to generate hydroxyl radicals, environmental remediation, biology, and life science. However, the slow Fe 3+ /Fe 2+ cycle and narrow applicable pH range still present significant challenges. Here, a heterostructured CoFe-layered double hydroxide/MoS 2 nanocomposite (CoFe-LDH/MoS 2 ) was prepared via simple electrostatic interactions. The heterostructure establishes a robust interfacial contact, leading to an abundance of exposed Mo 6+ sites. Consequently, the developed CoFe-LDH/MoS 2 +H 2 O 2 system exhibited superior performance in the degradation of tetracycline (>85%) within 60 min across a wide pH range from acidic to basic. Moreover, the CoFe-LDH/MoS 2 heterojunction catalysts exhibited exceptional resistance to common anions and efficiently degraded various organic pollutants. The mechanism study verified that the CoFe-LDH/MoS 2 had high efficiency in producing 1 O 2 and ‧OH to degrade various organic pollutants. The present study will serve as a foundation for creating efficient catalyst systems for related environmental remediation.
研究领域:
环境科学
·
催化材料
·
污染治理
✓ 已验证
DOI
PubMed
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2021
·Vol. 31
·期 51
·2107181
·
IF 18.808
Wen Zhang,Xue Jiang,Zemeng Dong,Jing Wang,Ning Zhang,Jie Liu,Guang-Rui Xu,Lei Wang
Modulating the morphology and chemical composition is an efficient strategy to enhance the catalytic activity for water splitting, since it is still a great challenge to develop a bifunctional catalyst for oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) over a wide pH range. Herein, Pd/NiFeO x nanosheets are synthesized with tightly arranged petal nanosheets and uniform mesoporous structure on nickel foam (NF). The porous 2D structure yields a larger surface area and exposes more active sites, facilitating water splitting at all pH values. The overpotential of Pd/NiFeO x nanosheets for OER is only 180, 169, and 310 mV in 1 m KOH, 0.5 m H 2 SO 4 , and 1 m phosphate-buffered saline (PBS) conditions at 10 mA cm −2 current density, as well as excellent HER activity with ultralow overpotential in a wide pH range. When using porous Pd/NiFeO x nanosheets as bifunctional catalysts for water splitting, it just required a cell voltage of 1.57 V to reach a current density of 20 mA cm −2 with nearly 100% faradic efficiency in alkaline conditions, which is much lower than that of benchmark Pt/CǁRuO 2 (1.76 V) couples, along with the improving stability benefiting from the good corrosion resistance of the inner NiFeO x nanosheets.
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Tianyu Zhang,Xiaoli Yan,Guangda Zhou,Kui Wang,Jingtao Zhang,Hua Zhang,Junjie Guo
Optimizing platinum-based catalysts for hydrogen generation via water electrolysis in pH-universal electrolytes is significant, and modulating the electronic structure is a viable strategy. Herein, platinum-iron (Pt–Fe) alloys with varying composition supported on carbon onions (CNOs) were successfully synthesized: Pt x Fe y @CNOs (x, y = 0.6, 0.4; 0.5, 0.5; 0.4, 0.6). Beneficial from the precisely modulated crystal plane spacing and electronic structure by tuning the Pt/Fe composition, in general pH electrolytes, Pt x Fe y @CNOs display outstanding hydrogen evolution reaction (HER) activity. The as-prepared Pt 0.5 Fe 0.5 @CNOs shows low overpotentials (η 10 ) of 11, 30, and 19 mV at −10 mA cm −2 in 0.5 M H 2 SO 4 , 1.0 M phosphate-buffered saline (PBS), and 1.0 M KOH electrolyte, respectively. Compared to commercial Pt/C, it displays enduring stability up to 24 h. Density functional theory (DFT) calculations indicate that Pt 0.5 Fe 0.5 @CNOs displays the lowest H* Gibbs free energy (ΔG H* ) and water dissociation energy values, due to the suitable proton adsorption and H 2 O dissociation processes offered by its electronic structure. Moreover, it is proven that the support with better wettability has a positive effect on HER performance of the catalyst. The optimal electronic structure and improved wettability provide novel insight into developing a Pt-based HER pH-universal catalyst.
研究领域:
材料科学
·
催化化学
·
理论计算
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Ranran Wei,Xiaoying Zhang,Min Yan,Xianlong Wang,Xuewen Wei,Runqi Zhang,Yinglong Wang,Liang Wang,Shuli Yin
Compared with layered materials such as graphite and transition metal disulfide compounds with highly anisotropic in-plane covalent bonds , it is inherently more challenging to obtain independent metallic two-dimensional films with atomic thickness. In this study, PtNi layered metallene nanobowls (LMBs) with multilayer atomic-scale nanosheets and bowl-like structures have been synthesized in one step using structural and electronic effects. The material has the advantage of catalyzing pH-universal hydrogen evolution reaction (HER). Compared with Pt/C, PtNi LMBs exhibited excellent HER activity and stability under all pH conditions. The overpotentials of 10 mA cm −2 at 0.5 M H 2 SO 4 , 1.0 M phosphate buffer and 1.0 M KOH were 14.8, 20.3, and 34.0 mV, respectively. Under acidic, neutral and alkaline conditions, the HER Faraday efficiencies reach 98.97%, 98.85%, and 99.04%, respectively. This study provides an example for the preparation of unique multilayer nanobowls, and also provides a basic research platform for the development of special HER materials.
研究领域:
材料科学
·
电化学
·
纳米技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ADVANCED MATERIALS
·
2021
·Vol. 33
·期 12
·2006965
·
IF 30.849
Yu-Lin Wu,Xiaofang Li,Yong-Sheng Wei,Zhaoming Fu,Wenbo Wei,Xin-Tao Wu,Qi-Long Zhu,Qiang Xu
The electrochemical hydrogen evolution reaction (HER) is an attractive technology for the mass production of hydrogen. Ru-based materials are promising electrocatalysts owing to the similar bonding strength with hydrogen but much lower cost than Pt catalysts. Herein, an ordered macroporous superstructure of N-doped nanoporous carbon anchored with the ultrafine Ru nanoclusters as electrocatalytic micro/nanoreactors is developed via the thermal pyrolysis of ordered macroporous single crystals of ZIF-8 accommodating Ru(III) ions. Benefiting from the highly interconnected reticular macro–nanospaces, this superstrucure affords unparalleled performance for pH-universal HER, with order of magnitude higher mass activity compared to the benchmark Pt/C. Notably, an exceptionally low overpotential of only 13 mV@10 mA cm −2 is required for HER in alkaline solution, with a low Tafel slope of 40.41 mV dec −1 and an ultrahigh turnover frequency value of 1.6 H 2 s −1 at 25 mV, greatly outperforming Pt/C. Furthermore, the hydrogen generation rates are almost twice those of Pt/C during practical overall alkaline water splitting. A solar-to-hydrogen system is also demonstrated to further promote the application. This research may open a new avenue for the development of advanced electrocatalytic micro/nanoreactors with controlled morphology and excellent performance for future energy applications.
研究领域:
材料科学
·
能源化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）