CARBON
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2020
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IF 8.821
Kunlin Liu,Ting Yang,Xuewen Zheng,Chengyang Wang,Mingming Chen
Low energy density is a fatal disadvantage of electric double-layer capacitor (EDLC). The improvement of the operation voltage of EDLCs is a more effective method to increase the energy density of EDLCs. When the operation voltage of EDLCs is higher than 2.7 V, the oxygen-containing functional groups on the surface of electrode materials (porous carbon) will decompose or chemically react with the electrolyte, causing significant deterioration of EDLC performance. In this paper, porous carbon with low oxygen content is prepared by using the potassium-assisted carbonization of chlorobenzene in Ar/H 2 mixed gas to improve withstanding voltage characteristic of porous carbon. By constructing a relatively closed and stable pyrolysis environment (employing the nickel crucible with a lid), using the carbonaceous precursor without oxygen atoms (chlorobenzene) and selecting reasonable carbonization operation atmosphere (Ar/H 2 ), the oxygen content of the as-prepared porous carbon (PC-KC-1000) is only 4.02 wt%. When the PC-KC-1000 sample is used as the electrode material of EDLCs, the operation voltage of EDLCs in the TEABF 4 /PC and EMIMBF 4 electrolytes is respectively 3.3 and 3.5 V, and the maximum energy density is respectively 53.5 and 64.4 Wh kg −1 . This strategy provides a new idea for the preparation of porous carbon with low oxygen content.
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Nano Research
·
2020
·Vol. 13
·期 12
·3206-3211
·
IF 8.183
Zhang Meng,Hu Zheng,Gu Lin,Zhang Qinghua,Zhang Linghui,Song Qian,Zhou Wei,Hu Shi
A series of carbon-based binary single-atom catalysts of Fe and Ni coordinated by nitrogen are fabricated using a glucose-chelating method. Depending on the Ni/Fe content, they exhibit a wide-range of controllable CO/H 2 ratio from 0.14 to 10.86, which is meaningful to specific chemical processes. The durability of the catalyst is evaluated over an 8-hour period with no significant degradation of activity. The variation of the faradaic efficiency with Ni/Fe content is justified by density-functional-theory based calculation of the reaction barrier in both hydrogen evolution and CO 2 reduction reactions.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2020
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IF 4.939
Jiayan Xue,Lizhen Long,Lin Zhang,Hongtian Luo,Li Yang,Fuchi Liu,Fengzhen Lv,Wenjie Kong,Jun Liu
Synergistic the modulation of photon absorption capability and interfacial charge transfer of the photocatalyst are highly required for developing high-performance heterojunction photocatalysts. The ternary CdS-graphene quantum dots-titanate nanotubes (CdS-GQDs-TNTs) nanocomposite have been prepared by an in situ growth method. The physicochemical characterization reveals that the GQDs are firmly decorated on both inner and outer surface of TNT through the formation of Ti–O–C chemical bonding, and CdS QDs are loaded on the outer surface of TNTs through strong interfacial interaction . The intimate integrated CdS-GQDs-TNTs nanocomposite exhibits much superior photocatalytic performance toward H 2 production compared with binary GQDs-TNTs and pure TNTs photocatalyst, which can be attributed to the combined interaction of the stronger visible light harvesting, the longer lifetime of photogenerated electron−hole pairs, faster interfacial charge transfer rate, fast and long-distance electron transport pass. The interfacial charge transfer mechanism of CdS-GQDs-TNTs ternary composite are proposed based on photoelectrochemical measurements.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2019
·
IF 4.084
Zhaohui Huang,Hui Chen,Lei Zhao,Xuan He,Yingying Du,Wei Fang,Weixin Li,Pan Tian
The development of ultraviolet to near-infrared (UV-Vis-NIR) responsive photocatalysts offers a unique opportunity for the full use of solar energy to solve the energy and the environmental problems. Here, successful preparation of a three-dimensional (3D) porous photocatalyst of graphitic carbon nitride quantum dot (CNQDs) modified g-C 3 N 4 /graphene oxide composite aerogel (CNGO/CNQDs) via hydrothermal and vacuum injection method was reported. In this unique ternary 3D photocatalyst, graphene oxide could improve the separation of photogenerated electrons and holes and promote the charge separation, while the aerogel's 3D network structure provided a rich active site. Simultaneously, due to the appropriate up-conversion performance of the nitrogen carbide quantum dots, CNGO/CNQDs achieved a light response from ultraviolet (UV) to near-infrared (NIR). These properties endow it with a good photocatalytic performance. The hydrogen production efficiency of CNGO/CNQDs reached 1231 μmol h −1 , which was 16 times more than that of matrix material . In addition, the apparent quantum yields (AQY) of CNGO/CNQDs at wavelengths of 420 nm and 700 nm were 13% and 0.116%, respectively.
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CHEMICAL ENGINEERING JOURNAL
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2019
·
IF 8.355
Yanglin Chen,Xueqing Liu,Ling Hou,Xiaorui Guo,Ruiwei Fu,Jianmin Sun
Photocatalytic water splitting for hydrogen production is a brilliant method for utilization of solar energy. Herein, a series of covalent bonding oxygen-doped carbon nitride/graphitic carbon nitride hybrids (O-CN/CN) have been synthesized via solvothermal treatment using cyanuric chloride, cyanuric acid (derived from hydrolysis of cyanuric chloride) and urea-derived graphitic carbon nitride as precursors. In O-CN/CN hybrids, guest O-CN was covalently bonded with incomplete polycondensation –NH x derived from the host CN surface as verified by XRD, FT-IR, XPS and solid-state 13 C MAS NMR spectra. With assistance of Pt co-catalyst, the most efficient O-CN/CN-3 photocatalyst showed the highest H 2 generation rate at 6.97 mmol g −1 h −1 under visible light irradiation (λ > 420 nm) by 12.4 times as that of pristine CN (0.56 mmol g −1 h −1 ). Moreover, the apparent quantum yield (AQY) was estimated as 21.4% at 425 nm irradiation for O-CN/CN-3. The improved photocatalytic performance was ascribed to the extended visible light absorption, the inhibited photo-induced charge carrier recombination and rapid charge carriers transfer that were confirmed by UV–vis diffuse reflectance spectra, photoluminescence spectra, transient photocurrent responses, electrochemical impedance spectroscopy and time-resolved photoluminescence. Moreover, the photocatalytic activity displayed unnoticeable deactivation within five recycles, further verifying that O-CN/CN hybrids were stable for visible-light-driven H 2 evolution. This present work promotes new insights into Z-scheme heterojunction engineering for graphitic carbon nitride.
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JOURNAL OF CATALYSIS
·
2026
·
IF 6
Chaosi Liu,Yijing Gao,Yixiang Niu,Yumei Zhang,Cheng Wang,Tengda Li,Chunhui Xu,Weidong Zhu,Xinqing Lu
Develop Pd-based catalysts for propylene epoxidation with H 2 and O 2. • Sn species in PdSn/Ti-MWW increase the electron density of Pd. • Increased electron density of Pd enhances the H 2 utilization. • Sn significantly promotes the catalytic propylene epoxidation. The low-temperature epoxidation of propylene with H 2 and O 2 to propylene oxide (PO), commonly referred to as the low-temperature HOPO process, over titanosilicate zeolite-supported Pd catalysts is economically attractive and environmentally friendly. However, PO selectivity remains a major challenge for these systems and is comparatively low, because this process is commonly accompanied with propylene hydrogenation to propane. In the present study, a novel and efficient Ti-MWW-supported PdSn catalyst (PdSn/Ti-MWW) was developed for this low-temperature HOPO process, displaying a substantially high PO selectivity. The results on extensive characterizations, in combination with Density Functional Theory (DFT) calculations, for PdSn/Ti-MWW and Pd/Ti-MWW verify that the introduction of Sn species into Pd/Ti-MWW can boost the electron density of Pd species while does not affect the coordination states of Ti species and the textural properties of the zeolite. Interestingly, the enhanced Pd electron density will weaken the adsorption of propylene on the Pd active sites, resulting in inhibiting propylene hydrogenation, which is beneficial for the selective production of PO. Catalytic tests reveal that the optimal 0.33Pd0.22Sn/Ti-MWW catalyst achieves a PO selectivity of 68.4 % and a maximum PO productivity of 7.5 mol g Pd -1 h −1 , far exceeding monometallic Pd/Ti-MWW, while the undesired propane selectivity drops sharply. Moreover, PdSn/Ti-MWW shows an excellent stability and reusability as key catalytic traits. Thus, this work establishes an effective electronic modulation strategy for designing high-performance bimetallic Pd catalysts, and lays solid experimental and theoretical foundations for the industrial application of sustainable low-temperature HOPO technology. Download: Download high-res image (81KB) Download: Download full-size image
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
·
IF 22.1
Chenxi Tang,Tengfei Bao,Shuming Li,Xiuyan Wang,Heng Rao,Ping She,Jun-sheng Qin
Metal sulfides have attracted extensive attention in photocatalysis , but are limited by the high combination rate of photo-induced charges due to their bulky structures. Herein, a bioinspired three-dimensional (3D) penetrating structured micro-mesoporous Z-scheme heterojunction of NiCoFe-layered double hydroxides@ZnIn 2 S 4 (NiCoFe-LDH@ZIS) with S vacancies was constructed. The NiCoFe-LDH@ZIS heterojunction was prepared by limiting the growth of ZIS through intercalating flower-like ZIS within dandelion-like LDH. The obtained NiCoFe-LDH@ZIS demonstrated a superior photocatalytic H 2 evolution (PHE) rate (113.57 mmol g −1 h −1 ) and 97.78 % conversion rate of benzylamine oxidation, simultaneously. This superior photocatalytic performance benefits from the enhanced charge separation induced by the combination of 3D penetrating micro-mesoporous structure, the introduction of S vacancies, and Z-scheme heterojunction. This dimensional-matched 3D penetrating porous heterojunction affords more abundant active sites, accelerated separation of photogenerated carriers, and reduced activation energy of H 2 evolution. This unique structure provides a feasible reference for bi-functional photocatalytic reactions.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
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IF 22.1
Xinlei Zhang,Fei Wu,Guicun Li,Lei Wang,Jianfeng Huang,Alan Meng,Zhenjiang Li
Photocatalytic water splitting is a prospective approach to address the energy and environmental challenges. Herein, an amorphous Ni@NiS x cocatalyst has been fabricated and simultaneously assembled onto CdS to form amorphous-crystalline Ni@NiS x -CdS photocatalyst via a partial reduction strategy. Comprehensive experiments and theoretical calculations demonstrate that the synergistic effects between the electronic coupling of amorphous-crystalline interface and the gradient work function variation induced by Ni nanocluster encapsulation achieve the deeper downshift of the S p-band center to optimize H* intermediate adsorption, enhance charge extraction ability though Schottky junction and lower H* adsorption Gibbs free energy (ΔG H* ). Accordingly, the optimal Ni@NiS x -CdS photocatalyst delivers a remarkable photocatalytic H 2 production rate of 78.7 mmol·g −1 ·h −1 with an apparent quantum efficiency (AQE) of 36.74% at 420 nm, which is approximately 18.3 and 1.5 times than that of CdS and NiS x -CdS, respectively. This work offers a novel insight into the development of amorphous nanocomposite cocatalysts for promoting solar-to-H 2 energy conversion.
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ChemSusChem
·
2023
·
IF 8.4
Juanjuan Han,Yangyang Zhang,Xiumeng Zheng,Yuyang Lu,Wanting Li,Xiaorong Zhou,Zhandong Ren,Yi Liu,Meixue Hu,Li Xiao,Lin Zhuang
Graphical A novel AEM with good strength and flexibility was synthesized by combining rigid PPO and flexible PVA. Dual cationic groups were added to improve ion concentration and create ion channels, enhancing ion conductivity. Cross-linking and phase separation improved the AEM's resistance to alkali. A series of cross-linked AEMs ( c -DQPPO/PVA) are synthesized by using rigid polyphenylene oxide and flexible poly(vinyl alcohol) as the backbones. Dual cations are grafted on the PPO backbone to improve the ion exchange capacity (IEC), while glutaraldehyde is introduced to enhance compatibility and reduce swelling ratio of AEMs. In addition to the enhanced mechanical properties resulting from the rigid-flexible cross-linked network, c -DQPPO/PVA AEMs also exhibit impressive ionic conductivity, which can be attributed to their high IEC, good hydrophilicity of PVA, and well-defined micro-morphology. Additionally, due to confined dimension behavior and ordered micro-morphology, c -DQPPO/PVA AEMs demonstrate excellent chemical stability. Specifically, c -DQPPO/PVA-7.5 exhibits a wet-state tensile strength of 12.5 MPa and an elongation at break of 53.0 % at 25 °C. Its OH − conductivity and swelling degree at 80 °C are measured to be 125.7 mS cm −1 and 8.2 %, respectively, with an IEC of 3.05 mmol g −1 . After 30 days in a 1 M NaOH solution at 80 °C, c -DQPPO/PVA-7.5 experiences degradation rates of 12.8 % for tensile strength, 27.4 % for elongation at break, 14.7 % for IEC, and 19.2 % for ion conductivity. With its excellent properties, c -DQPPO/PVA-7.5 exhibits a peak power density of 0.751 W cm −2 at 60 °C in an H 2 -O 2 fuel cell.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Qiong Liu,Liling Wei,Qiaoyue Xi,Yongqian Lei,Fuxian Wang
Solar-driven water splitting is a promising approach for H 2 generation, but in order to accelerate the reaction rate, high-cost sacrificial agents are usually required. Photoreforming of biomass serves as an alternative strategy for sustainable H 2 generation. Carbon nitride has recently emerged as a promising photocatalyst for the photorefoming reaction, however its performance is largely hindered by its poor visible light absorption. Here, we report, for the first time, the fabrication of an edge functionalized carbon nitride with remarkable visible light absorption via an in-situ C–N coupling method. By using N-acetylethanolamine (NA) as an additive to react with the precursors including urea, dicyandiamide, and melamine, the ethyl alcohol groups are grafted to the heptazine rings by replacing the terminal amino groups. Experimental results and DFT calculations reveal that the introduction of ethyl alcohol group leads to the generation of a new discrete energy level in the bandgap, resulting in significant increase in visible light absorption. The ethyl alcohol group herein serves as an electron donor, which would modulate the electron distribution to form an internal electric field to improve the charge separation. Moreover, the presence of ethyl alcohol group could favor the absorption of the biomass entity. The tuned CN shows superior photoreforming performance compared to the pristine CN in the presence of proton reduction Pt cocatalysts. It allows for visible-light-driven conversion of several monosaccharides into H 2 without the need for sacrificial agents.
研究领域:
材料科学
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光催化
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能源转换
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Journal of Materials Chemistry A
·
2023
·Vol. 12
·期 3
·1753-1763
·
IF 11.9
Yan Zhao,Yan Zhang,Qianqian Xu,Hanyu Gong,Mingyang Yan,Kaiyu Feng,Xiang Zhou,Xuefan Zhou,Dou Zhang
Hydrothermally synthesized Nd-doped bismuth titanate (Bi3.15Nd0.85Ti3O12, BIT-Nd) hierarchical microspheres with assembled nanosheets were developed for water splitting and wastewater purification utilizing the piezo-phototronic effect for the first time. Undoped Bi4Ti3O12 (BIT) microspheres were simultaneously studied for comparison to reveal the role of Nd doping. Under the combined light and ultrasound excitation, the degradation efficiency of RhB (C0 = 10 mg L−1) solution reached 97.5% in 8 minutes in the presence of the BIT-Nd microspheres, leading to an ultrahigh first-order rate constant k of 0.407 min−1, which was 4.9 times higher than that of the BIT microspheres. More impressively, superior piezo-photocatalytic activity in water splitting compared to that of other reported piezo-photocatalysts was achieved in the BIT-Nd microspheres, which showed a H2 evolution rate of 1330.3 μmol g−1 h−1 without any cocatalyst or scavenger. To understand the origins of the excellent piezo-photocatalytic performance, microstructure analysis and piezoelectric and photoelectric characterization, as well as density functional theory calculations were carried out. After Nd doping, the atomic framework of the Ti–O octahedron underwent an apparent distortion, resulting in a stronger ferroelectric polarization, and thus a larger piezoelectric potential output under pressure. Moreover, the thinner nanosheets in the BIT-Nd microspheres were more susceptible to deformation under the ultrasonic effect, which was also beneficial to generate a higher piezoelectric field that inhibited the charge carrier recombination. Additionally, the presence of Nd 4f orbitals in BIT-Nd effectively reduced the band gap and promoted the spectral absorption and production of photogenerated carriers. These merits enabled the BIT-Nd microspheres to exhibit strong piezo-photocatalytic activity.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2023
·
IF 8.2
Chuang Zhu,Fenfen Wei,Huibin Jiang,Zihan Lin,Lingyue Zhong,Yan Wu,Xiangjun Sun,Lihua Song
Horseradish peroxidase (HRP) is an enzyme that is widely used in various fields. In this study, the effects of molecular hydrogen (H 2 ) on the activity and structural characteristics of HRP were investigated by employing multiple spectroscopic techniques , atomic force microscopy (AFM) and molecular dynamics (MD) simulations. The results demonstrated that H 2 could enhance HRP activity, especially in 1.5 mg/L hydrogen-rich water (HRW). The structural analysis results showed that H 2 might alter HRP activity by affecting the active sites, secondary structure , hydrogen bonding network, C S groups, and morphological characteristics . The MD results also confirmed that H 2 could increase the Fe N bond distance in the active site, affect the secondary structure, and increase the number of hydrogen bonds . The MD results further suggested that H 2 could increase the number of salt bridges, and lengthen the S S bonds in HRP. This study primarily revealed the mechanism by which H 2 enhances the HRP activity, providing insight into the interactions between gas and macromolecular proteins. However, some of the results obtained via MD simulations still need to be verified experimentally. In addition, our study also provided a new convenient strategy to enhance enzyme activity .
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