Catalysts
·
2024
·Vol. 14
·期 8
·496
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IF 3.8
Kaige Zhao,Xinhao Xu,Manli Wang,Tao Chen,Qianlin Ju,Lulu Hao,Zelin Chen,Xiaolong Yu,Changjiu Li
The electrocatalytic oxidation of urea combined with wastewater splitting is considered a promising approach for sustainable hydrogen production, characterized by minimal energy consumption. However, its evolution is greatly hindered by the shortage of efficient and easily accessible electrocatalytic materials. Here, a facile electrochemical activation strategy was conceived and proposed to construct a Cu-doped NiOOH nanolayer encapsulated on Cu2O nanodendrites on Cu mesh substrate (Cu-NiOOH/Cu2O/CM) from the electrodeposited Ni/Cu2O/CM heterostructured precatalyst. It was verified that the incorporation of Cu not only facilitates the rapid formation of Ni(III)species but also contributes to the formation of Cu-Ni(III)bifunctional electrocatalytic active sites. Benefiting from the accessible Cu-Ni(III)dual active sites, high active surface area, good hydrophilic and aerophobic surface properties and superior electrical conductivity of the Cu mesh substrate, the as-prepared Cu-NiOOH/Cu2O/CM exhibits enhanced bifunctional electrocatalytic abilities for electrocatalytic urea oxidation reaction (UOR) and hydrogen evolution reaction (HER). Particularly, for the Cu-NiOOH/Cu2O/CM||Cu-NiOOH/Cu2O/CM configuration toward the UOR||HER coupled system, a significantly reduced cell voltage of 1.43 V vs. RHE @ 10 mA·cm−2was obtained. The observed cell voltage for the conventional overall water splitting is approximately 190 mV higher than that observed for overall urea splitting. This study proposes a viable approach to achieve and optimize the bifunctional UOR/HER performance of NiOOH active species, which holds significant importance for efficient and stable hydrogen generation from urea-contaminated substandard water.
研究领域:
材料科学
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电化学
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可再生能源
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DOI
高影响因子
JOURNAL OF NANOPARTICLE RESEARCH
·
2023
·Vol. 25
·期 8
·1-13
·
IF 2.5
Zhu Jiantao,Wen He,Han Wei,Ma Jiantai,Zhang Feng,Liu Chaowei
The growing concern about the environmental consequences of anthropogenic CO 2 emissions significantly stimulated the research of low-cost, efficient, and recyclable solid adsorbents of CO 2 capture. Metal–organic frameworks (MOFs) are a promising porous material for CO 2 adsorption. Hybrid materials consisting in copper benzene-1,3,5-tricarboxylate (Cu-BTC) and Cu doped graphitic-carbon nitride (Cu-g-C 3 N 4 ) were prepared through solvothermal method as CO 2 adsorbent. The size range of Cu-BTC@1.8%Cu-g-C 3 N 4 was 9.0 ~ 19.4 μm, which was lower than the size range of Cu-BTC (14.6 ~ 29.6 μm). The hybrid adsorbents had lower Brunauer–Emmett–Teller (BET) surface areas and pole volume due to the combination with Cu-g-C 3 N 4 . The CO 2 adsorption capacity of Cu-BTC@1.8%Cu-g-C 3 N 4 increased by 49.5% compared with that of pure Cu-BTC because of more adsorption sites including unsaturated metal centers and N atoms. Moreover, the Cu-BTC@1.8%Cu-g-C 3 N 4 had good stability in CO 2 adsorption capacity after multiple adsorption cycles. Graphical abstract
研究领域:
环境科学
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材料科学
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化学工程
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产品关联
DOI
高影响因子
Surfaces and Interfaces
·
2024
·
IF 5.7
Huiyu Tian,Haifeng En,Bingwen Li,Jinxian Zhao
An efficient Cu@C/SiO 2 catalyst for the hydrogenation of dimethyl oxalate (DMO) to methyl glycolate (MG) was prepared by sorbitol-modified ammonia evaporation method followed by calcination in N 2 . The Cu@C/SiO 2 catalyst exhibited the superior catalytic activity and stability for DMO hydrogenation compared with the Cu/SiO 2 catalyst. The optimized Cu@C/SiO 2 –1/4 catalyst exhibited an MG yield of 63 % during 90 h long-term evaluation under temperature of 210 °C, pressure of 1.9 MPa, WHSV of 1.25 g DMO ·g Cu -1 ·h -1 and H 2 /DMO of 150. The characterization results indicated that Cu dispersion can be significantly enhanced by the addition of an appropriate amount of sorbitol and the surface Cu 0 and Cu + species were effectively regulated by the amount of sorbitol. The catalytic activity of Cu@C/SiO 2 was linearly dependent on specific area of Cu + species under the sufficient specific area of Cu° for H 2 dissociation. In addition, the sorbitol–derived carbon species on the catalyst were also favorable for the enhanced stability owing to the suppression of Cu sintering.
研究领域:
催化化学
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材料科学
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产品关联
DOI
高影响因子
Nanomaterials
·
2020
·Vol. 10
·期 11
·2170
·
IF 4.324
Jialing Chen,Gang Peng,Tingyu Liang,Wenbo Zhang,Wei Zheng,Haoran Zhao,Li Guo,Xiaoqin Wu
The NH3-SCR activities and hydrothermal stabilities of fivexCu/MCM-22 zeolites with different Cu loadings (x= 2–10 wt%) prepared by incipient wetness impregnation method were systematically investigated. The physicochemical properties ofxCu/MCM-22 zeolites were analyzed by XRD, nitrogen physisorption, ICP-AES, SEM, NH3-TPD, UV-vis, H2-TPR and XPS experiments. The Cu species existing inxCu/MCM-22 are mainly isolated Cu2+, CuOxand unreducible copper species. The concentrations of both isolated Cu2+and CuOxspecies inxCu/MCM-22 increase with Cu contents, but the increment of CuOxspecies is more distinct, especially in high Cu loadings (>4 wt%). NH3-SCR experimental results demonstrated that the activity ofxCu/MCM-22 is sensitive to Cu content at low Cu loadings (≤4 wt%). When the Cu loading exceeds 4 wt%, the NH3-SCR activity ofxCu/MCM-22 is irrelevant to Cu content due to the severe pore blockage effects caused by aggregated CuOxspecies. Among the fivexCu/MCM-22 zeolites, 4Cu/MCM-22 with moderate Cu content has the best NH3-SCR performance, which displays higher than 80% NOxconversions in a wide temperature window (160–430 °C). Furthermore, the hydrothermal aging experiments (xCu/MCM-22 was treated at 750 °C for 10 h under 10% water vapor atmosphere) illustrated that all thexCu/MCM-22 zeolites exhibit high hydrothermal stability in NH3-SCR reactions.Keywords:Cu/MCM-22;NH3-SCR;Cu loading;hydrothermal aging
研究领域:
催化化学
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环境科学
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产品关联
DOI
PubMed
高影响因子
Environmental Science-Nano
·
2021
·Vol. 8
·期 9
·2618-2628
·
IF 8.131
Ting Chen,Zhiliang Zhu,Yujie Bao,Hua Zhang,Yanling Qiu,Daqiang Yin
The effective construction of electron transport channels has essential significance for electron-transfer rate enhancement in REDOX processes during peroxymonosulfate (PMS) activation. This study focuses on the establishment of Cu-involved covalent bonds due to the unique electron configuration of Cu ions. The strategy was achieved by anchoring Cu atoms to an O-doped g-C3N4 (Cu–O–CN) matrix. The C–O–Cu linkage was successfully constructed, derived from the precise incorporation of oxygen. From XAFS, H2-TPR, and solid-ESR characteristic observations, the desired REDOX performance was verified. The constructed C–O–Cu linkages were treated as electron transport channels for electron transfer while reacting with PMS, effectively accelerating the REDOX circulation of the Cu(II)/Cu(I) redox couple and promoting the consecutive generation of active species. Consequently, nearly 100% bisphenol A (BPA) was degraded in the Cu–O–CN/PMS reaction system within 30 min. This demonstrates the effectiveness of Cu–O–CN for PMS activation. The prepared Cu–O–CN exhibited definite stability and potential reusability. This research not only highlights the tailored design of heterogeneous catalysts for PMS activation but also broadens its application in water purification.
研究领域:
环境科学
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催化化学
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DOI
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-10
·
IF 14.7
Fan Yamei,Li Rongtan,Wang Beibei,Feng Xiaohui,Du Xiangze,Liu Chengxiang,Wang Fei,Liu Conghui,Dong Cui,Ning Yanxiao,Mu Rentao,Fu Qiang
Sintering of active metal species often happens during catalytic reactions, which requires redispersion in a reactive atmosphere at elevated temperatures to recover the activity. Herein, we report a simple method to redisperse sintered Cu catalysts via O 2 -H 2 O treatment at room temperature. In-situ spectroscopic characterizations reveal that H 2 O induces the formation of hydroxylated Cu species in humid O 2 , pushing surface diffusion of Cu atoms at room temperature. Further, surface OH groups formed on most hydroxylable support surfaces such as γ-Al 2 O 3 , SiO 2 , and CeO 2 in the humid atmosphere help to pull the mobile Cu species and enhance Cu redispersion. Both pushing and pulling effects of gaseous H 2 O promote the structural transformation of Cu aggregates into highly dispersed Cu species at room temperature, which exhibit enhanced activity in reverse water gas shift and preferential oxidation of carbon monoxide reactions. These findings highlight the important role of H 2 O in the dynamic structure evolution of supported metal nanocatalysts and lay the foundation for the regeneration of sintered catalysts under mild conditions.
研究领域:
催化
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材料科学
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化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CATALYSIS TODAY
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2019
·
IF 4.888
Yuhan Ma,Huawang Zhao,Cuijuan Zhang,Yingnan Zhao,Hong Chen,Yongdan Li
Cu-SSZ-13 is a highly active catalyst to remove NO x in the emission of diesel-powered engine. However, the enhancement of its stability in high-temperature (HT) hydrothermal conditions is a well-known challenge in application. This work presents a simple strategy to significantly improve its hydrothermal stability under HT hydrothermal condition by mechanically mixing another CHA type zeolite, Cu-SAPO-34. Both the two zeolites are synthesized via one-pot method, mixed in different ratios, and treated in 10% H 2 O/air at 750 °C for 16 h. The mixed samples are characterized before and after the hydrothermal treatment, and tested in NH 3 -SCR from 150 to 550 °C. The results show the activity of the hydrothermally treated catalysts increases with the increase of the amount of Cu-SAPO-34 up to 50 wt% in the mixed sample. The hydrothermal stability of Cu-SSZ-13 is obviously enhanced by mixing with Cu-SAPO-34. The dealumination is suppressed during the hydrothermal treatment; the framework and the isolated Cu 2+ sites are largely maintained in Cu-SSZ-13. This is attributed to the interaction between the two CHA zeolites during the hydrothermal treatment. We propose the delivery of extra-framework P species from Cu-SAPO-34 to Cu-SSZ-13 is critical to enhance the HT hydrothermal stability.
研究领域:
环境科学
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催化化学
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产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
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2023
·
IF 9.5
Qia Zhang,JianXiong Zou,Jin Ai,XiaoTian Pan,DongHong Qiao,Seong Chan Jun,Vijaykumar V. Jadhav,Ling Kang,Chun Huang,Jian Zhang
The current collector serves as a crucial element in supercapacitors, acting as a medium between the electrode material and the substrate. Due to its excellent conductivity, a metal collector is typically favored. Enhancing the binding strength between the collector and the substrate as well as between the collector and the electrode material has emerged as a critical factor for enhancing the capacitance performance. In this study, a Ag film with a grass root-like structure was initially grown on a PI substrate through the surface modification and ion exchange (SMIE) process. This Ag interlocking structure contributes to strong binding between the PI substrate and Ag without compromising the mechanical properties of the Ag film. To further enhance the electrochemical properties at low scan rates, electroless-plated Cu was subsequently deposited on the Ag film to form the Cu/Ag current collector. Moreover, the Cu within the Cu/Ag current collector served as a precursor for the growth of FeOOH–Cu(OH)2 via a two-step in situ method. The resulting FeOOH–Cu(OH)2/Cu/Ag structure as a whole is binder-free. Supercapacitors employing symmetric FeOOH–Cu(OH)2/Cu/Ag structures were assembled, and their energy storage properties were investigated. The solution-based low-temperature process used in this study offers the potential for cost-effective and large-scale applications.
研究领域:
材料科学
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能源存储
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DOI
PubMed
高影响因子
Journal of Energy Storage
·
2024
·
IF 8.9
Jianguo Duan,Xinshuai Yan,Kun Lei,Jianguo Cheng,Yaxiong Wang,Qingzong Su,Shimin Xu,Jianming Li,Qing Ma
The phase change materials (PCMs) are encapsulated into porous materials for collecting and storing heat energy has been widely used to overcome the intermittency of solar energy utilization. However, due to the inherent big pore structure and surface characteristics, metal porous materials are not ideal for PCM leakage-proof and slow photo-thermal response. To address these issues, A micro/nanostructured graphene-polyvinyl alcohol nanosheets/Cu(OH) 2 nanowire on a three-dimensional Cu foam (CF) to fill with PCM was designed and prepared. In the composite PCM, the polyvinyl alcohol/reduced graphene oxide (PRG) films coated on Cu(OH) 2 @Cu foam (CCF) provided a large number of active sites for the adsorption of modified paraffin wax (PWS). The prepared composite PCM has a stable structure and high thermal conductivity properties, meanwhile, the strong PRG films play a key role in enhancing leakage-proof and stability. The results show that the enthalpy value of PRG-CCF/PWS are 160.25 J·g −1 after 200 thermal cycles; which still maintains excellent cycle thermal reliability. In addition, under the simulated solar irradiation intensity is 120 mW·cm −2 , the heat storage rate and photo-thermal conversion efficiency of PRG-CCF/PWS are 1.37 J·s −1 and 90.25 %, respectively. It shows excellent photo-thermal response and uniform temperature distribution. This work provides an efficient, sustainable and affordable strategy for manufacturing high-performance composite PCM that can efficiently achieve solar energy utilization and energy management.
研究领域:
材料科学
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能源工程
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DOI
高影响因子
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
·
2023
·Vol. 120
·期 10
·e2206619120
·
IF 11.1
Wencui Li,Zhi Li,Hang Zhang,Pengxiao Liu,Zean Xie,Weiyu Song,Baijun Liu,Zhen Zhao
Selective oxidation of methane to organic oxygenates over metal–organic frameworks (MOFs) catalysts at low temperature is a challenging topic in the field of C1 chemistry because of the inferior stability of MOFs. Modifying the surface of Cu-BTC via hydrophobic polydimethylsiloxane (PDMS) at 235 °C under vacuum not only can dramatically improve its catalytic cycle stability in a liquid phase but also generate coordinatively unsaturated Cu(I) sites, which significantly enhances the catalytic activity of Cu-BTC catalyst. The results of spectroscopy characterizations and theoretical calculation proved that the coordinatively unsaturated Cu(I) sites made H2O2 dissociative into •OH, which formed Cu(II)-O active species by combining with coordinatively unsaturated Cu(I) sites for activating the C−H bond of methane. The high productivity of C1 oxygenates (CH3OH and CH3OOH) of 10.67 mmol gcat.−1h−1 with super high selectivity of 99.6% to C1 oxygenates was achieved over Cu-BTC-P-235 catalyst, and the catalyst possessed excellent reusability.
研究领域:
催化
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化学工程
·
材料科学
·
无机化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Sustainable Chemistry & Engineering
·
2020
·
IF 7.632
Qian Wang,Zhi Yu,Junting Feng,Paolo Fornasiero,Yufei He,Dianqing Li
The production of biofuel 2,5-dimethylfuran (DMF) from an important biomass platform of 5-hydroxymethyl furfural (HMF) involves a complicated reaction pathway due to the competition of C═O hydrogenation and C–O hydrogenolysis; however, the dependence of formed intermediates and catalytic sites needs to be further identified. Herein, we constructed a highly efficient and selective Cu/ZnO-Al2O3 catalyst via reduction of a CuZnAl-layer double hydroxide (LDH) precursor, aimed for studying the effect of Cu0/Cu+ species on forming different intermediates and their synergetic promotional effect on HMF hydrodeoxygenation. As expected, the dependence of formation of different intermediates on the Cu+/Cu0 ratio was observed; notably, Cu/ZnO-Al2O3 with higher Cu+/Cu0 ratio finally gave 90.1% DMF selectivity at 100% HMF conversion, more selective than CuNi/Al2O3 (59.6%) and Cu/MgO-Al2O3 (75.8%) references. By a combined study of in situ IR experiments, the observed correlation between the reaction intermediates and the Cu0/Cu+ site suggests that Cu0 tends to adsorb the C═O bond as well as hydrogen molecule, while the Cu+ site is preferable to adsorb and activate the C–O bond. With the synergy of dual active sites, the Cu/ZnO-Al2O3 catalyst showed both high activity and selectivity to DMF. This work provides deep insight into the nature of active Cu species in multiple functional group biomass platform transformation.
研究领域:
催化
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化学工程
·
生物化学
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材料科学
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产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2018
·
IF 11.698
Suqian Xu,Hanxu Zhu,Wenrui Cao,Zhibin Wen,Jinnan Wang,Corvini Philippe François-Xavier,Thomas Wintgens
Cu-Al 2 O 3 -g-C 3 N 4 and Cu-Al 2 O 3 -C-dots were synthesized for the first time to enhance the catalytic activity and utilization of H 2 O 2 . SEM, TEM, XPS, FT-IR, XRD, TPR and solid-state EPR were used to characterize the catalysts. In the Cu-Al 2 O 3 -g-C 3 N 4 system, the electron-rich centre of Cu and electron-deficient site of Al were formed due to the higher electronegativity of Cu. Moreover, Cu ions could coordinate with the hydroxyl on the tri-s-triazine ring of g-C 3 N 4 or the graphene conjugated π-domains of C-dots via the Cu O C linkage so that the orbital interactions involving electron transport from π → Cu also induced the formation of an electron-rich Cu centre and an electron-deficient π-electron conjugated system, resulting in the strengthening of the dual-reaction centres. This mechanism was validated by Roman, EPR and XPS spectra. In addition, EPR experiments demonstrated that two electron-transfer processes formed OH in the presence of H 2 O 2 . The first electron transfer was from the electron-rich Cu centres to H 2 O 2 , and the other was from H 2 O to the electron-deficient site. Thus, more OH were generated and high H 2 O 2 utilization was achieved in the Cu-Al 2 O 3 -g-C 3 N 4 and Cu-Al 2 O 3 -C-dots suspension. Furthermore, the turnover frequency (TOF) for the Cu-Al 2 O 3 -C-dots and Cu-Al 2 O 3 -g-C 3 N 4 dispersions were determined and were found to be much higher than those of the classic homogeneous Fenton reaction. Thus, Cu-Al 2 O 3 -g-C 3 N 4 and Cu-Al 2 O 3 -C-dots showed high activity and stability for the catalytic degradation of organic pollutants under mild conditions.
研究领域:
环境科学
·
材料科学
✓ 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）