ACS Sustainable Chemistry & Engineering
·
2021
·
IF 8.198
Fengyu Lai,Xiaodan Wang,Zheng Liu,Chao Wang,Hongxia Sun,Baoyou Geng
Silver catalysts play an irreplaceable role in the electroreduction of CO2 to CO. Here, we report the structure of bromide anion-adsorbed coral-like porous microspheres of silver (Ag BACPSs). They are formed by in situ electrolysis of AgBr microparticles (AgBr MPs) at a very low potential of −0.8 V (vs reversible hydrogen electrode (RHE)). Each AgBr MP is completely transformed into a porous coral-like microsphere, and the mass activity is greatly improved. Simultaneously, every microsphere has an interconnected open-pore structure, and all surfaces of the material adsorb bromide anions. The increased active electron density on the surface of the material helps the CO2 to obtain electrons on the surface of the electrocatalyst to form active species, which improves the selectivity of the catalytic material. Over a wide range of −0.4 to −0.9 V (vs RHE), the faradic efficiency for CO can be maintained above 91%, and the highest point can reach 98.7% at −0.6 V (vs RHE) in 0.5 M KHCO3 solution. In addition, it has excellent stability. The obtained catalyst material has good large-scale application prospects.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2024
·
IF 4.1
Zhuoshi Li,Yinhe Hai,Yibin Feng,Tong Guan,Tiantian Xiao,Jing Lv,Shouying Huang,Yue Wang,Xinbin Ma
Methyl glycolate (MG) is an important building block for synthesizing biodegradable material of polyglycolic acid. Hydrogenation of coal-based dimethyl oxalate (DMO) to MG is quite promising, where Ag-based catalysts exhibited excellent selectivity. Here, a series of Ag/SiO 2 -x catalysts with particle sizes of 1.4–13.5 nm were prepared, which showed significant structural sensitivity in DMO hydrogenation. For Ag nanoparticles of 1.4–2.7 nm, the turnover frequency (TOF) was linearly increased with the surface electron density of silver, but when the Ag nanoparticles further enlarged, no significant variation of TOF was observed. Combining DFT calculation and experimental results of the model catalyst, triangular nanoplate, it was deduced that the Ag (1 1 1) played a dominant role in DMO hydrogenation to MG, originating from the benefited MG desorption as well as promoted dissociation of H 2 and DMO. This understanding about Ag particle size effect may provide guidance for designing efficient catalysts for DMO hydrogenation to MG.
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2016
·
IF 8.328
Yuxi Gao,Anqi Duan,Shuang Liu,Xiaodong Wu,Wei Liu,Min Li,Shougang Chen,Xin Wang,Duan Weng
Three nanocubic Ag/Ce x Nd 1- x O 2 catalysts were synthesized to evaluate the influence of Nd doping on catalyst practicability. It was observed that Nd doping generated excessive ceria surface oxygen vacancies, but reduced the bulk oxygen vacancies . These variations in oxygen vacancies suppress the utilization of ceria bulk oxygen, and induce the formation of less active O 2− species instead of O 2 − , resulting in a low soot oxidation activity. However, the introduction of Nd can inhibit Ag sintering and thus enhance the catalysts’ thermal stability effectively. As a consequence, Ag/Ce 0.95 Nd 0.05 O 2 nanocubes make a good balance between the catalyst activity and stability. Moreover, it was observed that catalyst deactivation during soot oxidation becomes more obvious when the catalysts and soot are not in close contact.
研究领域:
催化化学
·
环境科学
·
材料科学
·
能源技术
·
大气污染防治
✓ 已验证
DOI
高影响因子
LANGMUIR
·
2024
·
IF 3.7
Tao Xue,Hui Li,Yuying Wang,Han Miao,Xinxin Li
Synthesizing catalyst supports with appropriate compositions and structures is crucial for reducing the sizes of metal nanoparticles and enhancing their catalytic activities. In this work, a series of monolithic hyper-cross-linked supports (HCP-CC) with hierarchical pores were synthesized. The monolithic structure facilitated easy operation in catalytic reactions, while the composition and structure of HCP-CC could be tailored simultaneously by utilizing the functional cross-linking agent cyanogen chloride. Furthermore, in situ loading of nano-Ag into HCP-CC resulted in the hybrid catalyst HCP-CC-Ag. The synergy of confinement and coordination effect controlled and limited the size of nano-Ag to approximately 3 nm, classifying them as ultrasmall nanoparticles, which ensured outstanding catalytic activity. This hybrid catalyst could improve the reaction rate constant to 0.423 min–1; it efficiently promoted the degradation of organic dye and exhibited great universality and recyclability, making it a potential heterogeneous catalyst for dye wastewater treatment.
研究领域:
催化材料
·
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Physical Chemistry C
·
2018
·
IF 4.484
Xueyan Chen,Min Chen,Guangzhi He,Fei Wang,Guangyan Xu,Yaobin Li,Changbin Zhang,Hong He
Ag-based catalysts are efficient materials for formaldehyde (HCHO) oxidation in the low-temperature range. It has been reported that K addition can increase the catalytic performance of Ag-based catalysts, whereas the specific role of K doping remains ambiguous. In this work, Ag/Al2O3 and K–Ag/Al2O3 catalysts with different K doping levels were prepared and subsequently tested for catalytic HCHO oxidation. It was observed that K doping has a dramatic promotion effect on the activity of the Ag/Al2O3 catalyst. The 2K–Ag/Al2O3 sample was the most active catalyst, over which HCHO could be completely converted into CO2 and H2O in a gas hourly space velocity of 100 000 mL/(gcat h) at 65 °C. The catalysts were next characterized by X-ray powder diffraction, Brunauer–Emmett–Teller, transmission electron microscopy, H2-temperature-programmed reduction, UV–vis, X-ray absorption fine structure, and in situ diffuse reflectance infrared Fourier transform spectroscopy methods. The characterization results show that addition of K species increased the content of metallic Ag species in Ag/Al2O3 catalysts and promoted the adsorption and activation of oxygen species, whereas excessive doping with K+ resulted in the agglomeration of Ag particles and loss of some metallic sites. Therefore, the 2K–Ag/Al2O3 catalyst demonstrated the best performance among the series of K-doped catalysts. Promotion of O2 activation by K doping, rather than enhanced Ag dispersion or surface OH activation or exposure of more Ag(111) facets, was found to be the key factor in the improved catalytic performance of K–Ag/Al2O3 catalysts.
研究领域:
环境催化
·
材料化学
·
大气污染控制
·
纳米催化
·
表面科学
✓ 已验证
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2018
·
IF 4.439
Mengyao Ouyang,Jian Wang,Bo Peng,Yujun Zhao,Shengping Wang,Xinbin Ma
A highly efficient Ag catalyst supported on a novel Ti-decorated spherical fibrous silica (Ag/Ti-KCC-1) was synthesized via a facile approach. Characterization of catalysts, including FT-IR, N 2 physisorption, TEM, ICP-OES and DRUV–vis was carried out to investigate the physicochemical properties of the catalyst, XPS, H 2 -TPR, H 2 -TPD and DMO-TGA were conducted to further elucidate the effect of Ti dopant. It is shown that the Ti additive is able to, (1) inhibit the aggregation of Ag; (2) induce electron transfer from Ti to Ag, which effect the Ag dispersion and the adsorption ability of the reactants on the catalyst surface. Proper amount of Ti additive provided a balanced coverage of both hydrogen and dimethyl oxalate (DMO) on catalyst surface, which is essential in promoting the performance of the catalyst in the hydrogenation of DMO. By using the novel 10Ag/0.02Ti-KCC-1 catalyst, a high MG yield of 93.0% under extremely high WHSV of 1.75 h −1 is achieved.
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
ENERGY CONVERSION AND MANAGEMENT
·
2024
·
IF 9.9
Si Li,Zhenchong Xiao,Yu Shi,Liang Zhang,Jun Li,Qian Fu,Xun Zhu,Qiang Liao
To realize the utilization of power energy from thermally regenerative batteries and treat flue gas, an eco-friendly coupled system of thermally regenerative battery-driven electrochemical reduction of carbon dioxide is proposed. This system recovers low-grade waste heat for electrical power while in-situ utilization for carbon dioxide reduction. The results show that carbon nanotubes-loaded silver catalyst enhances electrochemical carbon dioxide reduction performance due to increased active sites exposure. Output voltage and maximum power correlate linearly with the number of cell pairs in the thermally regenerative battery stack. Operating with 4 cell pairs, the eco-friendly coupled system achieves an average carbon monoxide Faradaic efficiency of 76.6 % and an average carbon monoxide Faradaic current density of 5.4 mA cm −2 . A minimum of 3 cell pairs is necessary for system operation. The increase of cell pairs in a certain range is beneficial for the performance improvement of electrochemical reduction of carbon dioxide. The eco-friendly coupled system attains an average Faradaic efficiency of 89.4 % and an average carbon monoxide Faradaic current density of 17.8 mA cm −2 with 8 cell pairs. This coupled system indicates a feasible and promising way to simultaneously reduce the emission of low-grade waste heat and carbon dioxide in flue gas without additional inputs.
研究领域:
环境科学
·
化学工程
·
能源技术
✓ 已验证
产品关联
DOI
高影响因子
Journal of Energy Chemistry
·
2025
·
IF 14.9
Min Zhang,Zengyi Tan,Mufan Xing,Yang Wang,Xun Zhu,Qian Fu
The scaling-up of electrochemical CO 2 reduction requires circumventing the CO 2 loss as carbonates under alkaline conditions. Zero-gap MEA cell configurations with a proton exchange membrane represent an alternative solution in a pure acidic system, but the catalyst layer in direct contact with the hydrated proton environment usually leads to H 2 evolution dominating. Herein, we show that polydimethyldiallyl-ammonium-chloride-coated Ag (Ag@PDDA) electrode exhibits outstanding performance with a FE of 86%, a single-pass conversion of 72%, and a stability of 28 h for CO production in pure-acid MEA compared with ammonium poly(N-methyl-piperidine-co-pterphenyl) decorated Ag (Ag/QAPPT) and cetyltrimethylammonium bromide decorated Ag (Ag/CTAB). The in situ ATR-SEIRAS reveal that PDDA creates a positive charge-rich protective outer layer and an N-rich hybrid inner layer, which not only suppresses the migration of H + during the electrolysis process and blocks the direct contact between H 2 O and Ag catalyst, but also promotes the generation from CO 2 to *COOH in a pure-acid system. This work highlights the importance of polyelectrolyte engineering in regulating the electrocatalytic interface and accelerates the development of proton exchange membrane CO 2 electrolysis.
研究领域:
电化学
·
环境科学
·
材料科学
·
化学工程
·
纳米技术
✓ 已验证
产品关联
DOI
高影响因子
Nature Communications
·
2025
·Vol. 16
·期 1
·1-10
·
IF 15.7
Liu Hong,Yu Yu,Bai Ye,Yang Yingchen,Wang Yaoxuan,Li Woyuan,Li Longhua,Hao Jinhui,Shi Weidong
The electrocatalytic reduction of carbon dioxide (CO 2 RR) to ethanol (C 2 H 5 OH) represents notable research significance and commercial value in large-scale chemical production. However, the limited selectivity for C 2 H 5 OH and the uncontrollable changes in active sites during reaction process restrict the ability of catalyst to achieve stable and efficient CO 2 RR to C 2 H 5 OH at industrial current density. Here, we report a system that immunizes the reconstruction of catalytic active sites, where the CuAg catalytic centers are protected by nitrilotriacetic acid (NTA). Importantly, the constructed CuAg@NTA catalyst exhibits low barriers for C-C coupling and hydrogenation of *CH 2 CHO to *CH 3 CH 2 O. Consequently, the catalyst achieves a high ethanol faradaic efficiency (FE C2H5OH ) of 87.21% with a partial current density of −218.03 mA cm −2 . Furthermore, the catalyst maintaining over 70% of FE C2H5OH after 300 h at −250 mA cm −2 , which are leading among previously reported catalysts in the selectivity and stability of CO 2 RR to C 2 H 5 OH at industrial current density. This study provides insights into the selectivity and stability enhancement of catalysts for electrocatalytic CO 2 RR to C 2 H 5 OH.
研究领域:
电催化
·
能量转换
·
材料科学
·
化学工程
·
环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Nature Catalysis
·
2019
·Vol. 2
·期 12
·1107-1114
·
IF 0
Li Zhe,Fu Jian-Yu,Feng Yi,Dong Cun-Ku,Liu Hui,Du Xi-Wen
Finding highly active and low-cost catalysts is a crucial endeavour to harvest clean hydrogen via electrochemical water splitting. Currently, the best catalyst for the hydrogen evolution reaction is based on metallic platinum whose high price severely restricts large-scale application. Here we report a silver catalyst with superior activity and durability in an acid medium that outperforms commercial platinum on carbon, especially under high applied voltages. We adopt a physical technique—laser ablation in liquid—to generate a high density of stacking faults in silver nanoparticles. We find that the stacking faults can cause a low coordination number and high tensile strain, which jointly improve the adsorption energy and transform the non-active silver into a highly active catalyst. In light of the high activity, conductivity, durability and low price, the silver catalyst can serve as a promising alternative to commercial platinum on carbon for industrial application.
研究领域:
催化
·
电化学
·
材料科学
·
能源材料
✓ 已验证
DOI
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Fengling Zheng,Jiang Gong,Hanqing Zhang,Weihan Shu,Xue Wang,Siqian Qin,Chuancai Zhang,Bin Dai
The Co-Ag x /TiO 2 catalysts with low mass content of Co and Ag were synthesized through the impregnation method and investigated for dimethyl oxalate (DMO) hydrogenation to methyl glycolate (MG). Remarkably, the Co-Ag 0.7 /TiO 2 catalyst with an Ag concentration of 0.7 wt%, exhibited an impressive yield of MG of ∼94.4 %, surpassing the yields of MG obtained with Co/TiO 2 (∼54 %) and Ag 0.7 /TiO 2 (∼69 %) catalysts. Various characterizations elucidated that the exceptional catalytic performance of Co-Ag 0.7 /TiO 2 can be ascribed to the synergy between Co and Ag, resulting in the formation of AgCoO 2 as high active site can improve the adsorption and activation of DMO and H 2 on catalyst surface. Additionally, the doping of a small amount of Ag regulated the contents of Lewis acidic and Brønsted acidic sites, leading to a high conversion of DMO and selectivity of MG. Furthermore, the excellent MG yield and long-term stability (at least 200 h) facilely obtained over our catalyst under mild reaction conditions guarantee a feasible prospect in the industrial application. This study not only unraveled the superior performance of the Co-Ag synergistic catalyst, but also carried significant implications for developing catalysts with low-content in DMO hydrogenation to MG.
研究领域:
催化
·
化学工程
·
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）