ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Chen Chen,Xianzhuo Lao,Junlong Li,Yidian Wang,Kuikui Wang,Dongxiang Li,Peizhi Guo
Pd-based nanocatalysts hold significant promise for application in alkaline direct ethanol fuel cells (DEFCs). To address the challenges of low Pd atom utilization and poor reaction kinetics in conventional Pd-based catalysts, a self-etching strategy has been developed to synthesize Pd3Pb1 nanoparticles (NPs) with tunable size and abundant tensile strain. The nanoparticles demonstrated a markedly enhanced electrocatalytic performance. Pd3Pb1 NPs-1 exhibited a current density of 2565 mA mgPd–1 for the ethanol oxidation reaction (EOR). Following self-etching, smaller Pd3Pb1 NPs-2 were synthesized, achieving a higher current density of 2820 mA mgPd–1 for EOR. Even after prolonged cyclic voltammetry (CV) testing, the Pd3Pb1 NPs-2 exhibited excellent stability. The high mass activity is attributed to a favorable balance between active intermediates and blocking species at the catalyst interface. This work presents a promising strategy for constructing nanocatalysts with tunable alloying degrees, offering highly efficient catalysts for fuel cell applications. Moreover, this study provides a reliable approach to preparing monodisperse nanocatalysts with controllable size and morphology through self-etching techniques.
研究领域:
材料科学
·
催化化学
·
能源科学
✓ 已验证
DOI
PubMed
高影响因子
ChemSusChem
·
2026
·Vol. 19
·期 1
·e202501680
·
IF 6.6
Jinlong Wu,Haiqiang Mu,Min Zhu,Xueru Zhao,Ting Zhang,Jiaxin Bai,Jin Zhang,Feng Li,Jing Li
Copper-based catalysts offer promise for CO 2 -to-C 2+ conversion but suffer from instability of Cu + species, which are active sites critical for enabling C−C coupling. In this work, we synthesized Lanthanum (La)-doped Cu x O (La-Cu x O) catalysts with varying La/Cu ratios to investigate how the interplay between doping-induced electronic effects and grain boundary (GB)-driven stabilization affects deep CO 2 reduction to C 2+ . Combined density functional theory calculations and in situ spectroscopic characterization reveal that the unique 4f orbital configuration and strong Lewis acidity facilitate charge transfer of La, stabilizing Cu + during CO 2 reduction reaction (CO 2 RR), while simultaneously inducing lattice distortion to increase GB density. This modulation preserves Cu + /Cu 0 interfaces while enhancing *CO dimerization kinetics. Furthermore, La doping boosts *CO coverage at GB-rich regions and lowers the C−C coupling barrier. The optimized La-Cu x O-2 catalyst (La/Cu = 0.224) achieves a 45.2% C 2 H 4 Faradaic efficiency (FE) and 75.4% C 2+ FE at −0.8 V RHE , with partial current densities of 87.5 and 146.7 mA cm −2 , respectively, surpassing undoped Cu x O. Remarkably, it retains more than 90% initial activity after 24 h operation, demonstrating exceptional stability. This work provides a rational strategy for stabilizing Cu + and tailoring pathways via rare-earth doping. Graphical La doping stabilizes Cu + /Cu 0 interfaces via electronic modulation and lattice distortion, enhancing grain boundary density in Cu x O catalysts for efficient CO 2 electroreduction. The optimized La-Cu x O-2 achieves 75.4% C 2+ Faradaic efficiency and 146.7 mA cm −2 partial current density at −0.8 V versus reversible hydrogen electrode, suppressing hydrogen evolution and enabling scalable CO 2 -to-C 2+ conversion.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ELECTROCHIMICA ACTA
·
2021
·
IF 6.901
Bao Liu,Chao Cai,Baopeng Yang,Kejun Chen,Yan Long,Qiyou Wang,Shuandi Wang,Guozhu Chen,Hongmei Li,Junhua Hu,Junwei Fu,Min Liu
Electrochemical carbon dioxide (CO 2 ) reduction reaction (CO 2 RR) to obtain C2/multi-carbon fuels is an appealing technology to reduce carbon emission and store intermittent renewable electricity. The C–C coupling process, as the most critical step for generating C2/multi-carbon fuels, strongly depends on the concentration of *CO intermediates around the active sites. In this work, we prepared porous copper nanospheres (P-Cu) that greatly improved the C–C coupling process by enriching *CO intermediates in the pore structure . The specific pore features of P-Cu were characterized in detail by scanning electron microscopy (SEM), transmission electron microscopy (TEM), and nitrogen adsorption/desorption tests. Obviously, the P-Cu exhibits higher specific surface area and richer pore structure than the control sample compact copper nanosphere (C-Cu). The CO gas sensor and temperature programmed desorption (TPD) tests prove that the P-Cu has better CO adsorption and enrichment capacity than C-Cu due to the rich pore structure. As a result, P-Cu exhibited a high C2 selectivity with a Faradaic efficiency (FE C2 ) of 57.22% at −1.3 V ( vs . RHE), which is about 2.5-fold than the C-Cu (FE C2 of 22.71%). This work provides an effective strategy to improve the activity and selectivity of C2 products in CO 2 RR by optimizing the adsorption/enrichment property of intermediates.
研究领域:
材料科学
·
能源化学
·
催化化学
✓ 已验证
DOI
高影响因子
ACS Catalysis
·
2023
·
IF 12.9
Yingying Cheng,Wenjing Xu,Jing Hou,Peng Kang
The electrosynthesis of multi-carbon chemicals such as glyoxylic acid (GX) and glycolic acid (GC) from oxalic acid (OA) offers a feasible pathway to achieve sustainable chemical production, especially when coupled with the electroreduction of CO2 to form OA. Here, we demonstrate a series of gallium tin oxide catalysts for selective, controlled OA electroreduction to GX and GC in acidic media. The product distribution can be tuned by changing the reaction temperatures. At room temperature using the GaSnOx/C catalyst, GX can be obtained with a GX Faradaic efficiency (FEGX) of 92.7% at −0.7 V vs RHE and a GX current density (jGX) of −100.2 mA cm–2. At a raised temperature of 80 °C using the GaSnOx/C catalyst, a GC Faradaic efficiency (FEGC) of 91.7% at −0.8 V vs RHE can be obtained. The accelerated OA electroreduction results from the Ga/Sn synergy in the catalysts. A proper Ga/Sn ratio not only enriches OA adsorption and enhances surface binding of intermediates, but also ensures catalyst stability in acidic media.
研究领域:
化学工程
·
材料科学
·
可持续化学
✓ 已验证
产品关联
DOI
高影响因子
CATALYSIS TODAY
·
2022
·
IF 6.562
Jia-Min Lyu,Shen Yu,Zhao Peng,Jian Zhou,Zhan Liu,Xiao-Yun Li,Yu-Li,Li-Hua Chen,Bao-Lian Su
Bifunctional catalysts are widely applied for many important reactions as the synergetic effect of two types of active sites remarkably improves catalysis performance. However, their bifunctionality has not been fully exploited since the proximity of bifunctional catalysts is hard to control. Herein, we demonstrate a bifunctional ZSM-5@Al 2 O 3 catalyst with a core-shell structure and a nano-scale proximity by in-situ growth of γ-Al 2 O 3 nanosheets on the surface of ZSM-5 crystals for methanol conversion. The nano-scale proximity endows the catalyst with higher reaction activity and C 2 –C 3 olefins yield (53 %) in comparison to the catalysts with micro-scale proximity (20 %) and millimeter-scale proximity (27 %), which can be attributed to the fluent transport of the reaction intermediates between two types of active sites. This strategy for constructing bifunctional catalysts with nano-scale proximity is conducive to understanding the relationship between proximity and catalytic performance in methanol conversion.
研究领域:
催化化学
·
材料科学
✓ 已验证
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Hongyu Chen,Zhaojie Wang,Xiaofei Wei,Siyuan Liu,Peng Guo,Peng Han,Haowei Wang,Jinbao Zhang,Xiaoqing Lu,Baojun Wei
Electrochemical reduction of CO 2 to C 2+ products is a sustainable energy-driven pursuit for high added-value hydrocarbons. Tremendous efforts have been made to copper based electrocatalysts, which are well-known for producing C 2+ products. However, being short of well-defined catalysts with stable Cu δ+ electronic structure hinders its practical application and in-depth understanding. Herein, we developed a facile one-pot approach to prepare Cu δ+ -rich catalyst by doping phosphorus. Enhanced performance and tunable product selectivities are achieved due to the electron donor–acceptor interaction based on phosphorus content in series. C 2 hydrocarbons and alcohols are produced with high (~44.9%) selectivity, in which C 2 H 4 (30.7 ± 0.9%) is dominant at −1.6 V vs reversible hydrogen electrode (RHE). This P-Cu catalyst shows a significantly higher current density (57.2 mA cm −2 ) compared to pristine Cu. In addition, the favorable Cu δ+ is reserved during CO 2 RR contributing to a long-term stability. Experimental results and DFT calculations demonstrate that the Cu δ+ moiety facilitates the adsorption of carbon intermediates, C-C coupling and hence promotes the generation of C 2 H 4 energetically. The well-designed catalyst indicates the profit of electronic structure engineering in designing catalysts for multiple-step chemical conversions.
研究领域:
材料科学
·
催化化学
·
能源化学
✓ 已验证
DOI
高影响因子
ACS Applied Nano Materials
·
2025
·
IF 5.5
Pengxuan Wu,Wanbing Ma,Yuxin Ge,Jinbao Xu,Minglei Lu,Xia Li,Liang Ma,Song Bai,Tiejun Wang
A facile one-step method was developed to promote the carbon dioxide reduction reaction (CRR) activities to form the C2 products (C2H4 and C2H5OH) via the capping agent and organic solvent-free involvement of copper (Cu) on graphitic carbon nitride (GCN). By tuning the using amount of the Cu precursor, Cu-GCN-0.2 exhibited a total Faradaic efficiency (FE) of more than 86.69 ± 0.73% for the C1 species (CO, CH4, HCOOH) and C2 species (C2H5OH, C2H4) as the CRR products when the electrolysis was carried out at an overpotential of 0.7 V (vs RHE) even after 12 h electrocatalysis and at a ratio of about 1:1 for C2/C1. Further investigation confirms that the enhanced CRR activities can be ascribed to three aspects: Firstl’y, smartl’y regulation of the Cu involvement during the synthesis of GCN created the CRR active site, which enables more CO2 to be adsorbed and activated at a lower overpotential to participate in the C–C couple procedures. Secondly, the neglected HER active site was formed when Cu was involved, which enables the well-maintained proton generation and adsorption activities for the proton-coupled electron transfer procedures, leading to the promoted C2/C1 ratio. Thirdly, the decreased electronic resistance accelerates the electronic transfer speed, which enables a faster reaction rate and a promoted long-term durability performance. This research provides a facile method for the rational construction and preparation of the electrocatalyst toward large-scale utilization in sustainable conversion and application.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
Journal of the American Chemical Society
·
2025
·
IF 15.6
Wen Yan,Tiantian Wu,Jia Liu,Zhe Zheng,Ming Ma
Electrolyte cation identity has been reported to influence the multicarbon (C2+) selectivity in CO2/CO electroreduction. However, most of the previous work for cation size effect is based on H-cell configurations, which may inadvertently distort the underlying mechanism of cation effect due to mass transport limitations, particularly for CO reduction. Here, using GDE-type flow electrolyzers, we report that the selectivity of total C2+ products on Cu is independent of alkali cation identity (Li+, Na+, K+, and Cs+) in the absence of the CO transport limitation. Notably, a high concentration of strongly hydrated cation (such as Li+) inhibits the total C2+ formation in CO reduction, whereas total C2+ selectivity is retained upon increasing concentrations of weakly hydrated cation (such as K+). Further investigations reveal that the CO coverage at a low cation concentration is almost independent of the cation identity, but the CO coverage at highly concentrated cations strongly relies on the alkali cation identity.
研究领域:
电化学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Catalysis Science & Technology
·
2023
·Vol. 13
·期 8
·2493-2499
·
IF 5
Junxing Wang,Fangwei Liu,Jianzhou Wu,Shihui Zou,Jie Fan
Engineering Mn–Na2WO4 catalysts for efficient oxidative coupling of methane (OCM) at low temperatures (T ≤ 700 °C) is appealing yet challenging. Herein, we report a LaCeZr ternary oxide supported Mn–Na2WO4 catalyst, which achieves 20.9% C2 yield at 700 °C with at least 50 hour stability. Characterizations suggest that LaCeZr ternary oxides can promote the redox properties of Mn–Na2WO4 catalysts, which facilitate O2 activation at low reaction temperatures and generate more active oxygen species to activate CH4 into C2 products.
研究领域:
化学工程
·
催化科学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Materials Chemistry A
·
2023
·Vol. 12
·期 2
·1218-1232
·
IF 11.9
Zi-Yang Zhang,Hao Tian,Han Jiao,Xin Wang,Lei Bian,Yuan Liu,Nithima Khaorapapong,Yusuke Yamauchi,Zhong-Li Wang
The electrochemical CO2 reduction reaction (CO2RR) for high value-added multi-carbon product (C2+) production over copper oxide-based catalysts is an important way to realize the carbon cycle. However, developing effective reaction interfaces and microenvironments to improve the Faraday efficiency (FE) and current density of C2+ remains a major challenge. Herein, we construct Cu0–Cu+–NH2 composite interfaces with the assistance of SiO2. Using Cu2O nanoparticles as a model catalyst, a layer of porous SiO2 is first coated on the surface of the particles, and then, a silane coupling agent containing –NH2 is bonded on the surface of SiO2. The strong interaction between SiO2 and Cu2O at the interface induces the oxidation effect of low valent Cu, and even under the CO2RR, part of Cu+ is reduced to Cu0 and part of Cu+ still maintains positive valence, forming the interface of Cu0–Cu+. SiO2 also acts as a bridge between copper species and –NH2 to create a Cu catalyst–NH2 group interface. With the help of the synergistic effect of the composite interfaces, the optimized Cu2O@SiO2–NH2 catalyst achieves a FE of 81.2% for C2+ products with a current density of 292 mA cm−2 at −1.7 V versus a reversible hydrogen electrode. In situ Raman and attenuate total reflectance-infrared absorption spectroscopy spectra show that the interaction between surface –NH2 and CO2 molecules enhances the adsorption and activation process of CO2 and promotes the formation of CO intermediates (*CO). On the Cu0–Cu+ interface, the C–C coupling process between *CO is accelerated, and the two interfaces synergistically promote the generation of C2+ products. This work provides a new strategy for constructing composite interfaces to improve the CO2RR to C2+ products.
研究领域:
电化学
·
材料科学
·
催化
·
可持续能源
✓ 已验证
DOI
高影响因子
MACROMOLECULAR CHEMISTRY AND PHYSICS
·
2016
·Vol. 217
·期 10
·1197-1204
·
IF 2.495
Jia Zhang,Wei Ji,Tian Liu,Chuanliang Feng
Syneresis property limits the further application of Kappa-carrageenan (κ-CG) in cell culture scaffold. To address this problem, κ-CG hydrogel is tailored by blending with a C2-symmetric benzene-based supramolecular gelator (B2). Scanning electron microscope (SEM) and Fourier transform infrared (FT-IR) spectroscopy confirm the semiinterpenetrating (semi-IPN) structure of the blended hydrogels and their wettability or thermal stability is also found to be improved. Based on the reduced syneresis, the growth and proliferation of the cultured HCT 116 cells on the blended hydrogels is enhanced compared with pure κ-CG hydrogels. This study paves an easy and feasible way to achieve stable and biocompatible κ-CG/B2 blended hydrogels with high water retention and it helps broaden the promising applications of κ-CG hydrogels in tissue engineering.
研究领域:
材料科学
·
生物医学工程
·
组织工程
✓ 已验证
DOI
高影响因子
ADVANCED MATERIALS
·
2026
·
IF 26.8
Kangwang Wang,Jie Zhan,Jun Liu,Zaichen Xiang,Wanyi Zhang,Lingyong Zeng,Kai Yan,Yan Sun,Huixia Luo
The photochemical CO 2 reduction reaction (CRR) represents a zero-carbon pathway for converting CO 2 into value-added chemicals, yet its industrial implementation has been constrained by low selectivity and product diversity. Dirac nodal arc semimetals characterized by ultrahigh carrier mobility (>25 000 cm 2 ·V −1 ·s −1 ) offer a promising platform to search for efficient catalysts for CO 2 conversion. Herein, we demonstrate that strategic Pt incorporation into PdSn 4 optimizes the electronic structure and carrier dynamics of this Dirac semimetal. Experimental and theoretical analyses reveal that the resulting Pd─Sn─Pt local electronic structure redistributes charge density around Pd and Pt atoms, which facilitates C─C coupling via *OC─COH and *OC─CHOH intermediates and enhances carrier mobility by 40% versus the pristine PdSn 4 single crystal. The optimized Pd 0.4 Pt 0.6 Sn 4 single crystal achieves C 2 H 4 i) formation rate of 328 µmol∙g −1 ∙h −1 ; ii) product selectivity of 73.1%; iii) electron-based selectivity of 89%. This work establishes electronic-structure-tunable Dirac semimetals as a new paradigm for multi-carbon photochemical CO 2 reduction, providing a design strategy for next-generation photocatalysts.
✓ 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）