Small
·
2019
·Vol. 16
·期 4
·1904964
·
IF 10.856
Zelin Chen,Yunwei Liu,Chang Liu,Jinfeng Zhang,Yanan Chen,Wenbin Hu,Yida Deng
The development of new type electrocatalysts with promising activity and antipoisoning ability is of great importance for electrocatalysis on alcohol oxidation. In this work, Pd nanowire (PdNW)/CuO x heterogeneous catalysts with different types of Pd O Cu interfaces (Pd/amorphous or crystalline CuO x ) are prepared via a two-step hydrothermal strategy followed by an air plasma treatment. Their interface-dependent performance on methanol and ethanol oxidation reaction (MOR and EOR) is clearly observed. The as-prepared PdNW/crystalline CuO x catalyst with 17.2 at% of Cu on the PdNW surface exhibits better MOR and EOR activity and stability, compared with that of PdNW/amorphous CuO x and pristine PdNW catalysts. Significantly, both the cycling tests and the chronoamperometric measurements reveal that the PdNW/crystalline CuO x catalyst yields excellent tolerance toward the possible intermediates including formaldehyde, formic acid, potassium carbonate, and carbon monoxide generated during the MOR process. The detailed analysis of their chemical state reveals that the enhanced activity and antipoison ability of the PdNW/crystalline CuO x catalyst originates from the electron-deficient Pd δ+ active sites which gradually turn into Pd 5 O 4 species during the MOR catalysis. The Pd 5 O 4 species can likely be stabilized by moderate crystalline CuO x decorated on the surface of PdNW due to the strong Pd O Cu interaction.
研究领域:
材料科学
·
电化学
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产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
·
IF 19.503
Min Chen,Jianhua Chen,Chuncheng Chen,Changbin Zhang,Hong He
Modification of TiO 2 with copper oxides clusters (CuO x -TiO 2 ) induces visible-light absorption and enhances its activity. In this work, we investigated the CuO x -anatase and CuO x -rutile for the photocatalytic oxidation of gaseous NH 3 under visible light. In contrast with the widely reported results that CuO x -anatase displays higher performance than CuO x -rutile in photocatalytic oxidation or reduction, we surprisingly observed that CuO x -rutile is able to oxidize NH 3 efficiently under visible light irradiation, while CuO x -anatase shows no activity. Further characterizations showed that visible-light inclines to drive the VB electrons of rutile TiO 2 to CuO x at the interface between rutile TiO 2 and CuO x , while it drives the electrons of CuO x to anatase TiO 2 at interface between anatase TiO 2 and CuO x . DFT calculations revealed that the interaction between CuO x and TiO 2 is markedly different in CuO x -anatase and CuO x -rutile, which induces the differences in the electronic distribution of interfacial Cu, O and Ti atoms, resulting in the distinct direction of charge transfer.
研究领域:
材料科学
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环境科学
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产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Hongjing Wang,Yanan Guo,Chunjie Li,Hongjie Yu,Kai Deng,Ziqiang Wang,Xiaonian Li,You Xu,Liang Wang
The artificial ammonia synthesis via electrochemical nitrate reduction has met increasing research interest, but it is still necessary to develop advanced catalysts with high nitrate-to-ammonia capability. Herein, we propose and demonstrate a one-step method to construct binder-free Cu foam-supported oxygen vacancy-rich Cu/CuOx in-plane heterostructured nanosheet arrays (Cu/CuOx/CF). In addition to exposing ample active sites, the two-dimensional nanosheet morphology greatly facilitates the mass/charge-transfer process during electrocatalysis. Besides, the in-plane heterojunctions and rich oxygen vacancies induced synergistic effect can modulate the electronic structure of active sites and thus tune the adsorption properties of the reactant intermediates and inhibit the formation of undesirable byproducts, which is conducive to the further improvement of nitrate reduction activity. As a result, these advantages endow the Cu/CuOx/CF with superior performance for ammonia synthesis via nitrate electroreduction, achieving high ammonia selectivity (95.00%) and Faradaic efficiency (93.58%).
研究领域:
材料科学
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电催化
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环境科学
✓ 已验证
DOI
高影响因子
ChemCatChem
·
2020
·Vol. 12
·期 6
·1639-1646
·
IF 4.853
Pan Li,Jianzhi Wang,Ning Cai,Lei Wang,Jing Tong,Faquan Yu
Graphical The center of attention : The CuO x @CoO nanorods grown on Cu Foam with the hierarchical configuration and the heterojunction interfaces enjoyed a couple of advantages of self-supported electrodes: needing no glue as an electrode, avoiding the agglomeration of MOFs-based particles, and forming the outward active figuration and large specific surface area. Those features lead to superior OER performances. The fabrication of cost-effective and performance-advanced electrocatalysts is in great requirements for water splitting to achieve sustainable oxygen production. A simple and effective precursor of ZIF-67 particles mounted on Cu(OH) 2 nanorods was induced by a template alignment method. After annealing, hierarchical CoO polyhedron-decorated CuO/Cu 2 O (CuO x ) nanorods on Cu foam (denoted as CuO x @CoO NRs/CF) were achieved, which displayed the heterojunction in CuO x components, hierarchical configuration and outward active sites. These features, verified by HRTEM, SEM, XPS and EDX, optimized the oxygen evolution reaction (OER) electrocatalyst. Benefiting from its large electrochemical surface area and the synergetic effect between CuO x and CoO, CuO x @CoO NRs/CF exhibited considerable catalytic activity with a low overpotential of 254 mV to obtain a current density of 10 mA cm −2 in alkaline electrolyte and a scarce loss of the initial catalyst activity over 24 h and over 5000 cycles. This work provides a channel to enhance the performance in OER.
研究领域:
材料科学
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电化学
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DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2025
·
IF 19
Kaiyang Xu,Chenyue Zhang,Lu Yang,Yaowen Xu,Binwen Zeng,Qian Chen,Bowen Li,Yang Zhao,Zhipeng Yu,Haoliang Huang,Wenlong Wang,Lecheng Liang,Shuqin Song,Lifeng Liu
Hybrid water electrolysis represents apromising approach for energy-efficient hydrogen (H 2 ) production. Herein, a highly active and selective electrocatalyst is reported for formaldehyde oxidation reaction (FOR), comprised of electrochemically deoxygenated copper nanosheet arrays supported on copper foam (D O -Cu-NS/CF). Comprehensive in-situ and ex-situ characterization confirms the formation of a Cu-rich, defect-abundant surface during deoxygenation. Using solid paraformaldehyde (p-HCHO) as anodic feedstock, D O -Cu-NS/CF achieves remarkable current densities of 500 and 963.3 mA cm −2 at low potentials of merely 0.199 and 0.495 V versus RHE, respectively. Theoretical simulations demonstrate that p-HCHO exists primarily as methane diolate anions (MDA) in alkaline media, and the lattice distortion in D O -Cu-NS/CF significantly enhances MDA adsorption and oxidative dehydrogenation, leading to outstanding FOR performance. A membrane electrode assembly (MEA) utilizing D O -Cu-NS/CF as the anode enables efficient bipolar H 2 production at 0.7 V for 280 h with a current density up to 500 mA cm −2 . This work highlights the crucial role of lattice engineering inenhancing FOR activity and offers new insights into the electrooxidation process of p-HCHO. The D O -Cu-NS/CF electrode developed shows significant potential for use as a cost-effective anode for energy-saving, high-rate production of H 2 through hybrid water electrolysis.
研究领域:
电化学
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能量转换
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材料科学
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纳米技术
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催化
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产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Tian Tang,Lyumeng Ye,Yanrong Chen,Jingyu Xue,Xiaoqiang Shen,Jinfei Chen,Fiona Hammond Quarcoo,Vladislav Rac,Vesna Rakić,Xinbao Li,Xuesen Du
The unique interface synergistic catalytic properties for metal oxide-supported catalysts have long been explored in several critical heterogeneous catalytic processes (e.g., CO oxidation reactions). However, interfacial synergistic catalysis is still a hitherto undescribed mechanism due to the lack of direct evidence at the atomic level. Thereinto, the CuO x -supported CeO 2 (CuO x /CeO 2 ) catalyst is a typical case. Herein, a combination study including representative theoretical calculations, in situ DRIFTS spectra and tailored molecular probe experiments supports a new carbonate-interface mediated Mars-van Krevelen (M−vK) mechanism for CO oxidation, i.e., CO molecules form carbonate intermediate species directly between spatial proximity (2.99 Å) double lattice oxygen sites with low oxygen vacancies formation energy (E form O v = 0.82 eV/0.83 eV) at the copper−ceria interface. The reaction energy barrier of this process is 0.32 eV, much lower than the 1.23 eV of the conventional M−vK mechanism. Besides, the spatial effect of double oxygen vacancies (O v ) generated by the depletion of intermediate carbonate species promotes the sustained and dynamic activation of O 2 , hence facilitating the efficient operation of the M−vK mechanism at low temperatures.
研究领域:
催化化学
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表面科学
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材料化学
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环境催化
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纳米催化
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DOI
高影响因子
Nano Research
·
2023
·Vol. 16
·期 7
·8827-8835
·
IF 9.9
Wang Xin,Miao Ming,Tang Bowen,Duan Haotian,Zhu Fulong,Zhang Huigang,Zhang Xian,Yin Wen-jin,Fu Yongzhu
Electrochemical conversion of CO 2 (CO 2 RR) into high-value fuel is identified as one of the promising approaches to achieve carbon neutrality. The synthesis of high-efficiency CO 2 reduction electrocatalysts with high C 2 :C 1 , selectivity remains a field of intense interest. Previous studies have shown that the presence of Cu(I) is beneficial for the reduction of CO 2 into C 2 products. However, the stable presence of Cu(I) remains controversial, especially in the negative potential window. Here we report a simple and easily scalable catalyst precursor Cu 2 (OH) 3 Cl/C, which automatically forms in-situ chlorine-doped Cu/Cu 2 O heterointerface during electrocatalysis. The catalyst not only exhibits a Faradaic efficiency of 33.03% but also provides a long-term stability of Cu + , gaining a stable electrolysis of 11 h, with an ethylene/methane ratio over 50. The experimental results and mechanistic studies confirm that the presence of Cl − inhibits the reduction of Cu + , inducing the formation of Cu 0 /Cu + , and reduces the reaction energy of the intermediate ⋆CO dimerization, thereby facilitating the formation of C 2 products. This work provides a feasible way to synthesize copper ions with long-term and stable positive charge in CO 2 RR and expands a new way to synthesize ethylene industrial products in the future.
研究领域:
材料科学
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电化学
·
催化反应
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产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Sheng Zhong,Bin He,Shuang Wei,Ruirui Wang,Ruirui Zhang,Ruixia Liu
Electrocatalytic glycerol oxidation reaction to produce high-value organic chemicals has research significance for managing the overproduction of glycerol and handling the energy crisis. Herein, a copper-based self-supporting catalytic electrode with a dynamic Fe-O-Cu optimized coordination (Fe-CuO x /CF) was prepared. The oxygen-bridged asymmetric coordination structure (Fe-O-Cu) optimized the electronic configuration and promoted the formation of the crucial intermediate species. After Fe was embedded in the lattice of copper oxides, a remarkable enhancement in the adsorption capacity of OH - and glycerol was confirmed. As a result, Fe-CuO x /CF exhibited an excellent production capacity of formate, with high faradaic efficiency and selectivity values of 93.65 % and 95.10 %. Concurrent production of formate and high purity hydrogen was achieved in the double-electrode flow electrolyzer. This work provides guiding significance for the optimization of the catalytic coordination and the design of high-efficiency transition metal-based catalysts for electrooxidation of biomass platform molecules.
研究领域:
电化学
·
催化材料
·
能源化学
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产品关联
DOI
高影响因子
Nanomaterials
·
2024
·Vol. 14
·期 23
·1930
·
IF 4.4
Sha Ni,Wenjing Wu,Zichao Yang,Min Zhang,Jianjun Yang
The Cu cocatalyst supported on the surface of TiO2photocatalysts has demonstrated unique activity and selectivity in photocatalytic CO2reduction. The valence state of copper significantly influences the catalytic process; however, due to the inherent instability of copper’s valence states, the precise role of different valence states in CO2reduction remains inadequately understood. In this study, CuOx/TiO2catalysts were synthesized using an in situ growth reduction method, and we investigated the impact of various valence copper species on CO2photocatalytic reduction. Our results indicate that Cu+and Cu0serve as primary active sites, with the selectivity for CH4and CO products during CO2photoreduction being closely related to their respective ratios on the catalyst surface. The adsorption and activation mechanisms of CO on both Cu+and Cu0surfaces are identified as critical factors determining product selectivity in photocatalytic processes. Furthermore, it is confirmed that Cu+primarily facilitates CH4production while Cu0is responsible for generating CO. This study provides valuable insights into developing highly selective photocatalysts.
研究领域:
材料科学
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环境科学
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产品关联
DOI
PubMed
高影响因子
Journal of Physical Chemistry C
·
2026
·
IF 3.4
Jiaying Liu,Shiwei Wang,Dong Wang,Zhihao Yu,Lin Zhu,Chunzheng Wu,Hongbo Yu
Modifying noble metal catalysts with transition metal oxides (MOx) is an effective strategy to enhance both catalytic activity and selectivity through interfacial synergy. However, achieving precise spatial colocalization of the metal and oxide phases remains a challenge. Herein, Pd1-(CuOx)1 hybrid nanostructures confined within KIT-6 mesoporous silica were rationally synthesized via in situ oxidative transformation of PdCu bimetallic nanoparticles (NPs) under controlled thermal treatment. The resulting Pd1-(CuOx)1/KIT-6 catalysts exhibited markedly enhanced activity and chemoselectivity for the hydrogenation of acetophenone to 1-phenylethanol compared with monometallic Pd/KIT-6 and PdCu/KIT-6. The optimal catalyst with a Pd/Cu molar ratio of 1:1 achieved 93.1% acetophenone conversion and 98.2% selectivity toward 1-phenylethanol, and demonstrated broad applicability across a range of ketone substrates. Comprehensive structural characterization revealed that the Pd-CuOx interfacial sites are central to the observed performance enhancement: metallic Pd facilitates H2 dissociation, while adjacent CuOx species are proposed to facilitate carbonyl adsorption, contributing to the overall synergistic enhancement. This interface-driven synergistic mechanism provides a general, efficient, and cost-effective strategy for the selective hydrogenation of multifunctional molecules.
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DOI
高影响因子
RSC Advances
·
2015
·Vol. 5
·期 40
·31708-31715
·
IF 3.84
Dongsheng Zhou,Zhiyuan Ren,Bo Li,Zhaoxia Ma,Xiaobin Zhang,Hangsheng Yang
Hexagonal boron nitride (hBN) was used as a CuOX/TiO2 catalyst carrier and its effect on NO reduction with NH3 was studied. After hBN was treated with concentrated HNO3, CuOX/TiO2 nanoparticles were dispersed well onto hBN, and the addition of hBN was found to promote NO oxidation, while at the same time suppress NH3 oxidation to NO, and thus promoted the selective catalytic reduction of NO at reaction temperatures between 150 to 350 °C, and a high de-NOX efficiency of 90.6% was achieved at 275 °C. Our study indicates that hBN is a promising catalyst promoter and carrier with excellent stability compared to carbonaceous materials.
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DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Juntong Liu,Ruoyu Sun,Yinsu Wu,Shengtao Xing
Adsorption is a cost-effective technology for the removal of refractory organic pollutants , and the regeneration of the spent adsorbent is crucial in terms of environmental and economic aspects. Herein, CuO X /MnFe 2 O 4 was synthesized by a two-step precipitation method and investigated as a peroxymonosulfate (PMS) catalyst for the regeneration of granular activated carbon (GAC) saturated with ofloxacin. The influences of reaction conditions on the regeneration of GAC with CuO X /MnFe 2 O 4 -PMS and the possible mechanism were explored. The results showed that CuO X /MnFe 2 O 4 exhibited high catalytic activity for the regeneration of GAC via the high mineralization of the adsorbed ofloxacin. Singlet oxygen was the dominant reactive species for organics removal, while O 2 •− and SO 4 •− also made a contribution to the degradation of organic intermediates. Under the optimized conditions, the regeneration efficiency of the spent GAC reached 98%, 89%, 87% and 85% for ofloxacin, ciprofloxacin, Orange II and methylene blue , respectively. Moreover, CuO X /MnFe 2 O 4 and GAC exhibited high stability and good reusability in this process, suggesting the potential application of this regeneration technology for removing refractory organic pollutants.
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DOI
高影响因子
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