Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 40
·23234-23242
·
IF 12.732
Hongyu Chen,Zhaojie Wang,Shoufu Cao,Siyuan Liu,Xiaojing Lin,Yi Zhang,Yizhu Shang,Qiuying Zhu,Sainan Zhou,Shuxian Wei,Baojun Wei,Daofeng Sun,Xiaoqing Lu
The electrocatalytic CO2 reduction reaction (CO2RR) on copper-based catalysts is a promising method to produce valuable chemicals, but its selectivity is much lower than expected largely due to insufficient research on the structure of new materials. Herein, the antimony-doped Cu/Cu2O (Cu/Cu2O–Sb) catalyst is developed for a highly selective CO2RR to CO. The synthesized Cu/Cu2O–Sb exhibits intensive suppression of hydrogen evolution, a low overpotential and high faradaic efficiency (FE) towards CO. The CO selectivity is as high as ∼95% with a partial current density of ∼6.3 mA cm−2 at −0.9 V and maintains over 90% in a broad range of potentials. DFT calculations reveal that the doping of antimony achieves the distinct activation of CO2 and suppression of hydrogen evolution. Meanwhile, the pre-adsorbed *CO significantly promotes the desorption of the neighboring *CO, which is the key for high selectivity of CO2RR to CO. This work will provide a new consideration for the origin of high selectivity during the CO2RR and pave the way toward design of highly selective CO2 reduction catalysts.
研究领域:
电化学
·
催化
·
材料科学
✓ 已验证
DOI
高影响因子
Small
·
2024
·
IF 13
Jing Gao,Yuan Gao,Jinghua Hao,Xiaolin Sun,Fuhua Zhao,Yuan Zhang,Wenyan Si,Jianfei Wu
All-solid-state lithium sulfide-based batteries (ASSLSBs) have drawn much attention due to their intrinsic safety and excellent performance in overcoming the polysulfide shuttle effect. However, the sluggish kinetics of Li 2 S cathode severely impede commercial utilization. Here, a Cu + , I − co-doping strategy is employed to activate the kinetics of Li 2 S to construct high-performance ASSLSBs. The electronic conductivity and Li-ion diffusion coefficient of the co-doped Li 2 S are increased by five and two orders of magnitude, respectively. Cu + as a redox medium greatly improves the reaction kinetics, which is supported by ex situ X-ray photoelectron spectroscopy. Density functional theory calculation (DFT) shows that Cu + , I − co-doping reduces the Li-ions diffusion energy barrier. The co-doped Li 2 S exhibits a remarkable improvement in capacity (1165.23 mAh g −1 (6.65 times that of pristine Li 2 S) at 0.02 C and 592.75 mAh g −1 at 2 C), and excellent cycling stability (84.58% capacity retention after 6200 cycles at 2 C) at room temperature. Moreover, an ASSLSB, fabricated with a lithium-free (Si─C) anode, obtains a high specific capacity of 1082.7 mAh g −1 at 0.05 C and 97% capacity retention after 400 cycles at 0.5 C. This work provides a broad prospect for the development of ASSLSBs with practical energy density exceeding that of traditional lithium-ion batteries.
研究领域:
材料科学
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电化学
·
电池技术
✓ 已验证
DOI
高影响因子
JOURNAL OF POWER SOURCES
·
2022
·
IF 9.794
Yixuan Zhang,Guoqiang Liu,Chang Su,Guangyin Liu,Hongda Sun,Danlei Qiao,Lei Wen
This work focuses on the improvement on the electrochemical performances of Fe–Mn based oxides as cathode for sodium ion batteries by doping Cu and F elements. The synthesized doped-compounds exhibit extremely excellent electrochemical performance. For instance, it's initial discharge capacity can reach 195.6 mAh g −1 at a current density of 10 mA g −1 . Meanwhile, after 200 cycles at 200 mA g −1 , it still remains a capacity of 124.1 mAh g −1 , 87.8% of the initial capacity of 141.3 mAh g −1 . More significantly, it can deliver a high capacity of 106.4 mAh g −1 at a high current density of 1000 mA g −1 . It is found that F/Cu co-substitution obviously improve the discharge capacity and cycle stability of Fe–Mn based oxide especially at higher current densities. Doping Cu and F elements has influence on the structure and morphology of the material, which results in the improvement of charge-discharge characteristics.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
DOI
高影响因子
AICHE JOURNAL
·
2019
·Vol. 66
·期 1
·e16746
·
IF 3.463
Chao Bian,Yin-Ning Zhou,Zheng-Hong Luo
Controlled radical polymerization (CRP) under external field has been an attractive research area in these years. In this work, a new electron transfer mechanism, that is, sonochemically induced electron transfer (SET) was introduced to mediate polymerization for the first time. The activator Cu I X/L complex was (re)generated from Cu II X 2 /L in dimethylsulfoxide (DMSO) by the SET process in the presence of free ligand tris(2-dimethylaminoethyl)amine (Me 6 TREN). The investigation of polymerization including the mechanistic insights and effect of experimental conditions on the rate of reaction has been undertaken. Kinetics of Cu(II)-catalyzed CRPs via SET under different conditions (i.e., Me 6 TREN concentration, catalyst loading, targeted degree of polymerization, and sonication power) were conducted in an unprecedentedly controlled manner, yielding polymers with predetermined molar masses and low dispersities ( Đ < 1.12). Attractively, the polymerization can be performed without the piezoelectric nanoparticles and exogenous reducing agent. Contamination by nonliving chains formed from sonochemically generated radicals is avoided as well. All of these results supported that Cu(II)-based catalyst activation enabled by ultrasonication has a promising potential in scale-up of CRP.
研究领域:
高分子化学
·
材料科学
·
化学工程
✓ 已验证
DOI
高影响因子
Nano Research
·
2023
·Vol. 17
·期 5
·4437-4443
·
IF 9.9
Zhong Junsen,Huang Bingkun,Yang Kunjie,Ma Zuju,Du Lingyu,Luo Ning,Tang Fengjiao,Hou Chuanxin,Jiang Fuyi,Kang Litao
The electrochromic (EC) mechanisms of inorganic materials are usually based on reversible cation insertion/extraction or metal deposition/dissolution, which are plagued by ion trapping and dendrite growth, respectively. In this paper, a novel conversion-type electrochromic mechanism is proposed, by making good use of the CuI/Cu redox couple. This CuI-based electrochromic system shows a neutral color switching from transparent and dim grey. By simply increasing the bleaching voltage, \({{\rm{I}}_3}^ - /{{\rm{I}}^ - }\) redox couple can be further activated. The generated \({{\rm{I}}_3}^ - \) will readily react with Cu, effectively improving the conversion reversibility and thereby rejuvenating the degraded electrochromic performance. Thanks to the well-designed electrode and the self-healing ability, this conversion electrochromic system achieves rapid response times ( t coloring : 23 s, t bleaching : 6 s), decant optical modulation amplitude (26.4%), high coloration efficiency (86.15 cm 2 ·C −1 ), admirable cyclic durability (without performance degradation after 480 cycles) and excellent optical memory ability (transmittance variation < 1% after 10 h open-circuit storage). The establishment of this conversion-type electrochromism may inspire the exploration of novel electrochromic materials and devices.
研究领域:
材料科学
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电化学
·
纳米技术
·
智能材料
·
能量存储与转换
✓ 已验证
DOI
高影响因子
Polymer Chemistry
·
2021
·Vol. 12
·期 30
·4347-4358
·
IF 5.582
Junnan He,Nan Zheng,Ming Li,YuBin Zheng,Wangze Song
Multicomponent polymerization has emerged as a promising strategy to develop functional polymers with versatile structures. In this work, a Cu-catalyzed four-component polymerization was developed using diynes, sulfonyl azides, nucleophiles, and a variety of electrophiles including alkyl glyoxylates, nitroalkenes, and Morita–Baylis–Hillman adducts to successfully synthesize a library of α-functionalized poly(N-sulfonylimidates)s with a wide substrate scope and high molecular weights (up to 20 000 g mol−1) in high yields (up to 86%). Such α-functionalized poly(N-sulfonylimidates)s could be further post-modified or utilized for the design of multi-functional and biodegradable polymers.
研究领域:
高分子化学
·
材料科学
✓ 已验证
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
Catalysis Science & Technology
·
2024
·
IF 4.4
Bin Guan,Junyan Chen,Zhongqi Zhuang,Lei Zhu,Zeren Ma,Xuehan Hu,Chenyu Zhu,Sikai Zhao,Kaiyou Shu,Hongtao Dang,Zhen Huang
As a significant technology of CO2 utilization, artificial CO2 photoreduction has received more and more attention. Herein, g-C3N4 catalysts modified with Bi and/or Cu for CO2 photothermal reduction were prepared by solvothermal synthesis and impregnation methods. Performance evaluation and physicochemical and photo- and thermochemical characterization indicated that Bi and Cu modification effectively enhanced the photo-absorption properties of g-C3N4 catalysts, improving charge transfer efficiency and catalytic performance. Compared with single-metal modification, Bi and Cu co-modification showed a narrower bandgap and more excellent light and CO2 absorption capacity, suggesting a certain synergistic effect of Bi and Cu co-modification. The alteration of the light absorption properties may be related to the surface plasmon effect of Bi and Cu, and the co-loading of Bi and Cu can exacerbate the effect, which can effectively enhance the photoresponsivity of the catalysts, leading to higher catalytic performance.
研究领域:
催化
·
材料科学
·
环境科学
·
化学工程
✓ 已验证
DOI
高影响因子
Journal of Macromolecular Science Part A-Pure and Applied Chemistry
·
2024
·
IF 2.1
Ping Jiang,Wan Liu,Jing Li,Yuan Gao
Straw and chitosan are underutilized raw materials, which could make a significant contribution to sustainable development. Herein, a novel chitosan-based hydrogel incorporating rice straw cellulose micro-fibrils (SCMF) was prepared to effectively remove Cu(II). FTIR and SEM showed that straw cellulose-g-poly (acrylic acid)/chitosan-g-poly (acrylic acid) interpenetrating polymer networks were prepared and the hydrogel SCCH had a 3D porous structure after cross-linking with AA. The swelling properties of SCCH were studied and compared in various pH solution. The results indicated that SCCH replayed pH responsibility, which had the largest and smallest swelling capacity at pH9.18 and pH4.00 respectively. The pseudo-second-order kinetic model can be effectively used to evaluate swelling kinetics of hydrogels. The effects of contact time and initial concentration on Cu(II) ion removal were investigated. The equilibrium adsorption capacity (Qe) was 209.2 mg/g and the obtained results indicated that the adsorption kinetics conformed to the pseudo-second-order. Chemical adsorption combined with porous physical adsorption endowed SCCH excellent swelling and adsorption properties. Tensile, compression, bending and twisting test convinced that SCMF played a significant role on the improvement of mechanical strength. This novel 3D porous chitosan-based hydrogel was identified to be a promising sorbent with advantages of excellent sorption and mechanical properties.
研究领域:
环境科学
·
高分子科学
·
材料工程
·
化学工程
·
可持续发展
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Zhen Li,Kailin Luo,Geng Zhang,Lingxuan Qian,Xiaodong Huang
Li metal is promising as the anode for next-generation Li-ion batteries; however, uncontrollable dendrite growth and severe side reactions between the Li metal and electrolyte greatly restrict its commercialization. Here, a 3D porous protective layer constructed by core@shell-Cu@Li 3 N particles is developed to solve the above issues. This protective layer is easily prepared just by one-step dip coating in Cu(NO 3 ) 2 /N-methyl-2-pyrrolidone (NMP) solution. Due to rapid Li + transport and good wettability of the protective layer, it effectively modulates Li + flux and thus homogenizes Li deposition. More importantly, as confirmed by both the experimental results and phase-field simulations, the 3D porous protective layer enforces the Li dendrite to laterally grow to form an interconnected network, which causes that the subsequent Li deposition is constrained and filled in the inner space rather than savage growth. Therefore, both the symmetric battery and full cell constructed by the protected Li electrode displays much longer lifespan than the one with bare Li even in unstable liquid carbonate electrolyte. Also, this protective layer is demonstrated to be compatible with Li 1+x Al x Ti 2−x (PO 4 ) 3 (LATP) solid-state electrolyte by suppressing the side reactions. This work paves a new and facile strategy for developing high-performance Li metal anode.
研究领域:
材料科学
·
电化学
·
电池技术
✓ 已验证
DOI
高影响因子
RSC Advances
·
2023
·Vol. 13
·期 20
·13902-13910
·
IF 3.9
Jing Tian,Weixin Qian,Haitao Zhang,Hongfang Ma,Weiyong Ying
In this paper, catalysts with different aluminum contents were prepared by a co-precipitation method using LDHs (layered double hydroxides) as the precursors through the adjustment of Cu2+ : Fe2+, and the catalysts were named LDO catalysts. The effect of aluminum on CO2 hydrogenation to methanol was investigated by evaluating the characterization. With the addition of Al, Ar physisorption results showed an increase in BET-specific surface area, TEM demonstrated a decrease in catalyst particle diameter, XRD showed that Cu and Fe existed in the catalyst mainly in the form of CuFe2O4 and CuO, XPS demonstrated a decrease in electron cloud density and an increase in base sites and oxygen vacancies, and CO2-TPD and H2-TPD results indicated that Al promoted the dissociation and adsorption of CO2 and H2. When the reaction temperature was 230 °C, the pressure was 4 MPa, H2/CO2 = 2.5 and the space velocity was 2000 ml (h gcat)−1, the best conversion (14.87%) and the highest methanol selectivity (39.53%) of the catalyst were obtained at 30% aluminum content.
研究领域:
催化
·
化学工程
·
材料科学
✓ 已验证
DOI
PubMed
高影响因子
BIOSENSORS & BIOELECTRONICS
·
2022
·
IF 12.545
Siyu Luo,Fanglei Liu,Siyu Gu,Ke Chen,Guohai Yang,Yingqiu Gu,Juntao Cao,Lu-Lu Qu
Food-borne pathogens are one of the leading causes of food poisoning, which vigorously affect food safety and human health. Therefore, the development of early and rapid detection methods for food pollution evaluation is the key to food safety and quality control. Herein, a simple and inexpensive photoelectrochemical (PEC) sensor is developed for highly selective and ultrasensitive detection of Staphylococcus aureus (S. aureus). The technique is based on “signal-off” that employs Cu–C 3 N 4 –TiO 2 heterostructures as photoactive materials and monolayer Cu–C 3 N 4 nanozyme as a signal amplifier. In the presence of S. aureus , the aptamer-modified Cu–C 3 N 4 (Cu–C 3 N 4 @Apt, a signal amplifier) and S. aureus were specifically anchored on the surface of the ligand-modified photoelectrode . The Cu–C 3 N 4 @Apt nanozyme acted as a peroxidase to catalyze the oxidation of 4-chloro-1-naphthol (4-CN) to produce insoluble precipitate on the electrode surface and resulted in a significant decrease in photocurrent . Based on the signal-amplification by the Cu–C 3 N 4 @Apt nanozyme, the constructed PEC sensor demonstrated a wide linear range between 10–10 8 CFU/mL for the S. aureus detection with the detection limit (LOD) as low as 3.40 CFU/mL. Furthermore, the PEC sensor was capable of determining S. aureus in spiked orange juice and milk, with the recovery of 91%–113%, indicating the reliability of the sensor for S. aureus detection in real samples. This investigation provides a feasible strategy for the design of highly selective and ultrasensitive PEC sensors to determine analytes in complex systems.
研究领域:
分析化学
·
生物传感器
·
食品安全
·
纳米技术
·
光电化学
✓ 已验证
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）