Carbon Neutrality
·
2024
·Vol. 3
·期 1
·1-20
·
IF 0
Guo Yafei,Gao Yuxuan,Guo Benshuai,Luo Yangna,Zhao Guoyang,Sun Jian,Li Weiling,Wang Ruilin,Zhao Chuanwen
Electrochemical CO 2 reduction (ECR) to value-added products is regarded as a sustainable strategy to mitigate global warming and energy crisis, and designing highly efficient and robust catalysts is essential. In this work, transition metal sulfides (TMS)-decorated CuS microflower-like structures were prepared via the one-pot hydrothermal synthesis method for ECR to CO, and the influence of TMS doping on ECR performance was demonstrated. Characterization of the catalysts was performed using XRD, FESEM-EDS, N 2 physisorption, and XPS, revealing the successful loading of TMS, the formation of microflower-like architectures and the generation of sulfur vacancies. Electrochemical tests demonstrated that doping ZnS, Bi 2 S 3 , CdS and MoS 2 improved the intrinsic CO 2 reduction activity of the CuS catalyst. Particularly, the MoS 2 -CuS composite catalyst with imperfect petal-like structure showed uniform distribution of edge Mo sites, which worked synergistically with the formed grain boundaries (GBs) and undercoordinated S vacancy sites in promoting CO 2 activation, stabilizing * COOH adsorption, facilitating * CO desorption, and lowering the energy barrier of the potential-limiting step for improved CO selectivity. The MoS 2 -CuS catalyst achieved a maximum CO selectivity of 83.2% at –0.6 V versus the reversible hydrogen electrode (RHE) and a high CO cathodic energetic efficiency of 100%. At this potential, the catalyst maintained stable catalytic activity and CO selectivity during a 333-min electrolysis process. The findings will offer a promising avenue for the development of efficient and stable catalysts for CO production from ECR.
研究领域:
材料科学
·
环境科学
·
能源化学
✓ 已验证
DOI
ENERGY & FUELS
·
2016
·
IF 2.835
Jing Zhang,Hui-hui Xu,Ying-zhou Lu,Hong Meng,Chun-xi Li,Biao-hua Chen,Zhi-gang Lei
A hyper cross-linked ionic polymer (HCIP) PVimBCmBn was synthesized through free radical polymerization of 1-vinylimidazole (Vim) and quaternized cross-linking with 1,4-bis(chloromethyl) benzene (BCmBn). Its composition, structure, morphology, specific area, porous structure and thermal stability were characterized, and the desulfurization performance was investigated. The results show that the HCIP prepared with stoichiometric ratio of PVim and BCmBn are ultrafine powders with specific area of 99.6 m2·g–1 and average pore size of 16.1 nm, being micro/mesoporous materials. The S-removability of HCIP is superior to its precursor (ethyl imidazole) and the imidazolium-based ionic liquids (ILs), which manifests the importance of the available micropores for the accommodation of sulfur molecules with less energy barrier. The adsorption isotherms of PVimBCmBn follow the Langmuir equation with its saturated adsorbance being 7.0, 5.2, and 4.1 mgS·g–1, respectively, for dibenzothiophene, benzothiophene, and thiophene in model oil at 293 K. However, its adsorptive removal ability for DBT in diesel oil is quite low due to its limited S-selectivity with respect to the abundant confused ring aromatics wherein.
研究领域:
化学工程
·
材料科学
✓ 已验证
DOI
高影响因子
JOURNAL OF ENVIRONMENTAL ENGINEERING
·
2024
·Vol. 150
·期 8
·04024038
·
IF 1.6
Jingcheng Wei,Jing Zhang,Bingyan Zhu,Tingfeng Xue,Zejia Song,Sumin Li,Liwei Pan
Activation of peroxymonosulfate (PMS) by catalysts for water treatment is very important for the sulfate radicals-based advanced oxidation technology. Constructing affordable and recyclable transition metal catalysts with high efficiency is highly desirable, but still challenging. In this study, a novel CoAl2O4/Co2O3@γ-Al2O3 catalyst for the activation of PMS was prepared with an excessive impregnation method, and its performance on the catalytic degradation of phenol in water was investigated. The composition and structure of the catalyst were characterized by X-ray diffraction, X-ray photoelectron spectroscopy, Fourier transform infrared spectroscopy, and N2 adsorption-desorption experiments. It was found that the catalyst could greatly promote the phenol mineralization in water as the total organic carbon removal increased from 4.27% to 57.64% after 60 min of reaction. The presence of Cl− inhibited the catalytic degradation of phenol in water at low concentrations, but promoted the catalytic degradation at high concentrations. However, HCO3− and CO32− revealed inhibitory effects on the catalytic degradation because they could scavenge free radicals in the system. Based on the electron spin resonance technique and the quenching experiments, O12 and SO4−· were identified to be the primary reactive species for the catalytic degradation. The CoAl2O4/Co2O3@γ-Al2O3 could be easily recovered and reused. The toxicity evaluation verified that the toxicity of the treated water was greatly decreased after the catalytic degradation. Therefore, the CoAl2O4/Co2O3@γ-Al2O3 prepared in this study could be an effective catalyst for the catalytic degradation of phenol in water by activating PMS.
研究领域:
环境科学
·
催化化学
✓ 已验证
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2019
·
IF 3.375
Jianfeng Fan,Mengwen Yan,Jiarong Huang,Liming Cao,Yukun Chen
To expand the application of shape memory materials in situations where elevated temperature and corrosion resistance are required, novel heat-triggered shape memory (HSM) fluorosilicon thermoplastic vulcanizates (TPVs) were designed via core–shell dynamic vulcanization. When the fluororubber (FKM)/silicone rubber (SR) ratio reached 1:1, excellent shape fixity (Rf ∼ 96%) and shape recovery ratios (Rr ∼ 98%) were achieved at the suitable switching transition temperature (Ttrans) of 160 °C. The influence of core–shell structure on shape memory behavior mainly comes from the following aspects: the improvement of interfacial compatibility promoting stress delivery between polyvinylidene fluoride (PVDF) and SR/FKM phases in the shape fixing and shape recovery process and the reduced number-average rubber particle size caused by the appropriate interfacial compatibility facilitating the increasing of interface area, which improved the nucleation density and induced abundant tiny crystals in the blends. Additionally, the formation of core–shell structure also endowed the TPVs with improved mechanical properties.
研究领域:
高分子材料科学
·
功能材料
·
智能材料
·
形状记忆聚合物
·
复合材料工程
✓ 已验证
DOI
高影响因子
JOURNAL OF POWER SOURCES
·
2016
·
IF 6.333
Zihao Li,Xiaogang Li,Youhao Liao,Xiaoping Li,Weishan Li
We report a novel composite of sulfur loaded in micropore-rich carbon aerogel (CA-S), as cathode of lithium-sulfur battery. Carbon aerogel (CA) is synthesized through phenol-formaldehyde reaction with a low catalyst concentration and carbonization under high temperature, and loaded with sulfur via chemical deposition and heat treatment. The physical properties of the resulting CA and the electrochemical performances of the resulting CA-S are investigated by scanning electron microscopy, thermal gravimetric analysis , Brunauer-Emmett-Teller characterization, electrochemical impedance spectroscopy , and galvanostatic discharge/charge test, with a comparison of a common carbon material, acetylene black (AB), and sulfur loaded in AB (AB-S). It is found that the CA is micropore-rich with micropore volume over 66% of total pore volume , and the CA-S exhibits significantly improved cyclic stability compared with AB-S. The improved performance of CA-S is attributed to the confinement of the micropores in CA to small sulfur allotropes and corresponding lithium sulfides.
研究领域:
电化学
·
能源材料
·
纳米材料
·
储能技术
✓ 已验证
DOI
高影响因子
Small
·
2018
·Vol. 14
·期 11
·1703279
·
IF 9.598
Qian Wang,Minghui Yang,Zhen-Bo Wang,Chao Li,Da-Ming Gu
Shuttle effect of the dissolved intermediates is regarded as the primary cause that leads to fast capacity degradation of Li–S battery. Herein, a microporous carbon-coated sulfur composite with novel rambutan shape (R-S@MPC) is synthesized from microporous carbon-coated rambutan-like zinc sulfide (R-ZnS@MPC), via an in situ oxidation process. The R-ZnS is employed as both template and sulfur precursor. The carbon frame of R-S@MPC composite possesses three kinds of pores that are distinctly separated from each other in space and are endowed with the exclusive functions. The central macropore serves as buffer pool to accommodate the dissolved lithium polysulfides (LPSs) and volumetric variation during cycling. The marginal straight-through mesoporous, connected with the central macropore, takes the responsibility of sulfur storage. The micropores, evenly distributed in the outer carbon shell of the as-synthesized R-S@MPC, enable the blockage of LPSs. These pores are expected to perform their respective single function, and collaborate synergistically to suppress the sulfur loss. Therefore, it delivers an outstanding cycling stability, decay rate of 0.013% cycle −1 after 500 cycles at 1 C, when the sulfur loading is kept at 4 mg cm −2 .
研究领域:
材料科学
·
电化学
·
能源存储
·
纳米材料
·
功能材料
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Jing Zhang,Caiyin You,Jian Wang,Hong Xu,Chuanzhi Zhu,Shaohua Guo,Weihua Zhang,Rong Yang,Yunhua Xu
For the practical application of lithium-sulfur batteries, the high areal capacity based on high loading sulfur cathode is urgently pursued. Herein, the electrochemical rate and cycling performance are significantly enhanced by the design of polar hierarchical-porous carbon container to confine sulfur species. The as-fabricated carbon container shows the following merits: providing an affordable pore volume of 4.94 cm 3 g −1 for confining sulfur and releasing volume changes; facilitating rapid electron/ion transfer pathway; allowing efficient chemisorption of polysulfides by polar active sites synergistically. As a result, the cathode displays a high rate capacity of 581 mA h g −1 at 8 C and a stable cyclability at 2 C. Importantly, the cathode with 7.2 mg cm −2 sulfur loading presents a high areal capacity of 9.75 mA h cm −2 at 0.05 C and high rate performance. Up to 7.5 mg cm −2 , the high loading cathode could still display a high areal capacity of 5 mA h cm −2 at 1 C after 80 cycles. Moreover, the container can successfully work in a pouch cell with low E/S ratio. These results show a promising way to promote the practical utilization of Li-S batteries.
研究领域:
材料科学
·
电化学
·
能源存储
·
纳米材料
·
功能碳材料
✓ 已验证
DOI
高影响因子
DALTON TRANSACTIONS
·
2024
·Vol. 53
·期 42
·17200-17206
·
IF 3.5
Wang Zhao,Jiazheng Zhou,Linan Wang,Wenqi Jin,Yingying Kong,Yu Chu,Junjie Li
Pb-based chalcogenides display abundant structural diversity and distinguished properties. Based on a mixed anion and dimensional reduction combined strategy, a wide band gap Pb-based thiohalide, Pb6Ba3Si2S8I10, has been rationally designed and synthesized experimentally by the flux method. The compound crystallizes in the Rc space group with cell parameters a = 9.7925(2) Å, b = 9.7925(2) Å, and c = 70.628(3) Å and is composed of [SiS4] tetrahedra and unprecedented [PbI5S2] polyhedral units, resulting in a unique quasi-two-dimensional structure, which enriches the chemical and structural diversity of Pb-based thiohalides. The experimental band gap of Pb6Ba3Si2S8I10 was determined to be 2.80 eV. Based on statistical analyses and to the best of our knowledge, it is the largest experimental optical band gap among the known Pb-based thiohalides. The results demonstrate the feasibility of using highly electropositive Ba atoms to regulate the dimensions of the structural framework of thiohalides and give new insights into the structure and property modifications of thiohalides by the mixed anion and dimensional reduction combined strategy.
研究领域:
无机化学
·
材料科学
·
固体化学
·
功能材料
·
半导体物理
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2015
·
IF 4.321
Wen Li,Ping-xiao Wu,Yajie Zhu,Zhu-jian Huang,Yong-hong Lu,Yue-wu Li,Zhi Dang,Neng-wu Zhu
In this study, CoMnAl mixed metal oxides (CoMnAl-MMO) were prepared and employed in heterogeneous activation of Oxone for bisphenol A (BPA) degradation. Typically, 10 mg L −1 of BPA could be completely degraded under the coexistence of 0.02 g L −1 of CoMnAl-MMO and 0.15 g L −1 of Oxone within 90 min at 25 °C. The degradation performance was evaluated in view of metal leaching and various effects, e.g., pH, Oxone dosage and temperature. The results indicated that the system of MMO/Oxone was suitable for the treatment of wastewater and presented favorable recycling and stability in both neutral and alkaline conditions. It was confirmed that BPA degradation catalyzed by CoMnAl-MMO followed well with the first order kinetics model and the an activation energy was calculated as 76.83 kJ mol −1 . The sulfate radicals were recognized as the main species to oxidize pollutants in the MMO/Oxone system. Particular attention was paid to the catalysis activation mechanism of peroxymonosulfate and the degradation pathway of BPA, which were analyzed by X-ray diffraction (XRD) and X-ray photoelectron spectroscopic (XPS), LC–MS and GC–MS.
研究领域:
环境科学
·
化学工程
·
材料科学
✓ 已验证
DOI
高影响因子
WATER RESEARCH
·
2015
·
IF 5.528
Junhe Lu,Jinwei Wu,Yuefei Ji,Deyang Kong
Sulfate radicals ( S O 4 − · ) are applied to degrade various organic pollutants. Due to its high oxidative potential, S O 4 − · is presumed to be able to transform bromide to reactive bromine species that can react with natural organic matter subsequently to form brominated products including brominated disinfection by-products (Br-DBPs). This research was designed to investigate the transformation of bromide in thermo activated persulfate oxidation process in the presence of humic acid (HA). Significant formation of bromoform and bromoacetic acids was verified. Their formation was attributed to the reactions of HA and reactive bromine species including Br·, B r 2 − · HOBr − , and free bromine resulted from the oxidation of bromide by S O 4 − · . Yields of Br-DBPs increased monotonically at persulfate concentration of 1.0 mM and working temperature of 70 °C. However, the time-depended formation exhibited an increasing and the decreasing profile when persulfate was 5.0 mM, suggesting further degradation of organic bromine. HPLC/ICP-MS analysis demonstrated that the organic bromine was eventually transformed to bromate at this condition. Thus, a transformation scheme was proposed in which the bromine could be recycled multiple times between inorganic bromide and organic bromine before being finally transformed to bromate. This is the first study that reveals the comprehensive transformation map of bromine in S O 4 − · based reaction systems, which should be taken into consideration when such technologies are used to eliminate contamination in real practice.
研究领域:
环境科学
·
水处理工程
✓ 已验证
DOI
高影响因子
JOURNAL OF POWER SOURCES
·
2019
·
IF 7.467
Liming Jin,Jie Ni,Chao Shen,Fenglai Peng,Qiang Wu,Donghao Ye,Junsheng Zheng,Gaoran Li,Cunman Zhang,Zhoupeng Li,Jim P. Zheng
A metallically conductive TiB 2 is developed to construct multifunctional separator toward improved lithium-sulfur (Li–S) battery performance. Coupled with two-dimensional graphene, the obtained TiB 2 @G separator fulfills a synergistic combination of strong physical and chemical sulfur immobilization as well as a high-efficiency sulfur reutilization, thus establishing a robust barrier against the polysulfide shuttling and enabling a fast and durable sulfur electrochemistry . As a result, cells based on TiB 2 @G separator exhibit a high sulfur utilization with 1350 mA h g −1 capacity at 0.05C, superb rate capability up to 5.0C, and excellent cyclability with a high capacity retention over 85% after 300 cycles at 0.5C. Moreover, significantly mitigated self-discharge and considerably high areal capacity of 5.8 mA h cm −2 can be also achieved, indicating the great promise of this separator design for the development of high-performance Li–S batteries.
研究领域:
电化学
·
能源材料
·
纳米材料科学
·
储能技术
·
电池化学
✓ 已验证
DOI
高影响因子
JOURNAL OF SOLID STATE CHEMISTRY
·
2017
·
IF 2.299
Yuan-Zi Xu,Cheng-Zong Yuan,Xue-Ping Chen
To design highly efficient and low-cost electrocatalysts for oxygen evolution reaction (OER) is a great challenge for electrochemical water splitting. Here we introduce a simple and cost-effective strategy for one-step synthesis of a three-dimensional Ni 3 S 2 /MoS X (x is close to 3) nanosheets on Ni foam (NF) via a sovelthermal reaction. The electrochemical performance of the Ni 3 S 2 /MoS X nanosheets on NF has been investigated and exhibits superior OER electrocatalytic activity as well as excellent electrochemical durability. As a novel non-noble-metal OER catalyst operating in basic electrolytes, this 3D cathode exhibits an onset overpotential of as low as 165 mV, a Tafel slope of 67.5 mV dec −1 and remarkable long-term stability. This catalyst maintains its catalytic activity for at least 14 h and only affords 50, 100, and 150 mA cm −2 OER current densities at overpotentials of 215 mV, 265 mV and 305 mV respectively.
研究领域:
材料科学
·
电化学
·
能源化学
·
纳米科技
·
催化化学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）