ADVANCED MATERIALS
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2024
·
IF 27.4
Yibo Xu,Shirong Wang,Hongli Liu,Xianggao Li
Organic metal halide perovskite solar cells (PSCs) bearing both high efficiency and durability are predominantly challenged by inadequate crystallinity of perovskite. Herein, a polymer microencapsulation-expansion-contraction strategy is proposed for the first time to optimize the crystallization behavior of perovskite, typically by adeptly harnessing the swelling and deswelling characteristics of poly(4-acryloylmorpholine) (poly(4-AcM)) network on PbI 2 surface. It can effectively retard the crystallization rate of perovskite, permitting meliorative crystallinity featured by increased grain size from 0.74 to 1.32 µm and reduced trap density from 1.12 × 10 16 to 2.56 × 10 15 cm −3 . Moreover, profiting from the protection of poly(4-AcM) microencapsulation layer, the degradation of the perovskite is markedly suppressed. Resultant PSCs gain a robust power conversion efficiency (PCE) of 24.04%. Typically, they maintain 91% of their initial PCE for 13 008 h in a desiccated ambient environment and retain 92% PCE after storage for 4000 h with a relative humidity of 50 ± 10%, which is the state-of-the-art long-term stability among the reported contributions.
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ACS Applied Materials & Interfaces
·
2015
·
IF 6.723
Zu-Sheng Huang,Xu-Feng Zang,Tao Hua,Lingyun Wang,Herbert Meier,Derong Cao
Five novel metal-free organic dyes DQ1–5 containing a dipentyldithieno[3,2-f:2′,3′-h]quinoxaline (DPQ) unit were synthesized and applied in dye-sensitized solar cells (DSSCs), where DPQ was employed as a π-spacer for the first time. Their photophysical, electrochemical, and theoretical calculations and photovoltaic properties were systematically investigated. All the five dyes show broad photoresponse. Especially the absorption edges of DQ3–5 extend to 800 nm on the TiO2 films. The inserted electron-rich unit 3,4-ethylenedioxythiophene or electron-withdrawing group benzothiadiazole (BTD) in DPQ-based dyes can greatly influence the optoelectronic properties of the dyes. In addition, the different electron donors also significantly affect the performance of the DSSCs. Under standard global AM 1.5 solar light conditions, the DQ5 sensitized solar cell obtained a power conversion efficiency of 7.12%. The result indicates that the rigid DPQ-based organic dye is a promising candidate for efficient DSSCs.
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Molecular Catalysis
·
2019
·
IF 2.938
Qiaoyun Liu,Fei Liu,Yaru Zhang,Yang Su,Aiqin Wang,Tao Zhang
A highly active and robust catalyst composed of Ru nanoparticles highly dispersed on zeolite H-beta was developed for transforming furfural into 3-acetyl-1-propanol (3-AP) in good yield (81%)under mild conditions (80 °C, 1 MPa H 2 ). Both the support nature and the preparation methods had significant impacts on the dispersion of Ru, eventually on the yield of 3-AP. Ion-exchange method proved best for obtaining the highly active and selective catalyst for this reaction. Moreover, the catalyst can be regenerated easily by calcination and reduction. This catalyst was further explored for the one-pot conversion of xylose and xylan to 3-AP with a yield of 46% and 31%, respectively, thus opening a new feasible pathway from biomass to valuable fine chemicals.
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ACS Catalysis
·
2025
·
IF 13.1
Yufeng Li,Jinbiao Yuan,Yunxuan Ji,Siyang Yan,Jiaxu Liu,Bing Liu,Xiaohao Liu
Developing efficient and stable catalysts to convert CO2 to desirable C1 products is of great importance for carbon resource utilization. Cobalt-based catalysts usually show high activity in methanation but poor selectivity to CO from the reverse water-gas shift (RWGS) reaction. Herein, we synthesized In-doped CeO2-supported cobalt catalysts for RWGS reaction, which achieved almost reverse 100% selectivity toward CO with a near-equilibrium CO2 conversion of about 49% at 500 °C and 1 MPa. Results showed that catalyst reduction could result in In species migration onto Co particles to form an InCo alloy, thereby modulating the cobalt electronic structure. It thus strengthened Co–H* bonding but weakened CO adsorption and activation, in turn inhibiting CH4 formation via HCOO* and CO hydrogenation. Interestingly, the reaction temperature-dependent deactivation was observed over 10Co/CeO2, owing to cobalt oxidation determined by the O atom chemical potential (μO). Theoretical investigations demonstrate that μO is related to the free energy of H2O and H2 (μO = GH2O‐GH2), where the reaction temperature exhibits different degrees of effect on GH2OandGH2. Based on the deactivation behavior study, we successfully developed a simple strategy to suppress oxidation deactivation by mixing with hydrophilic H-ZSM-5 zeolite to drive H2O desorption away from the cobalt surface during the CO2 methanation reaction with much more H2O molecules produced.
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JOURNAL OF STRUCTURAL CHEMISTRY
·
2025
·Vol. 66
·期 1
·1-15
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IF 1.4
Ma X.,Yang Y.,Zhou J.,Li Z.,Hong X.,Jin S.,Wang D.
Preparation, X-ray crystal structure, Fourier transform infrared (FTIR) spectroscopy, and elemental analysis of complexes 1 , 2 from the pyridine and the mono- and dicarboxylic acids are reported. XRD and FTIR analysis demonstrate that both belong to the organic salt. The salt 1 crystallizes in the triclinic, space group \(P\bar{1}\) , with a = 7.271(3) Å, b = 9.548(4) Å, c = 14.698(7) Å, α = 78.435(6)°, β = 85.975(7)°, γ = 71.492(6)°, V = 948.0(8) Å 3 , Z = 2. The salt 2 crystallizes in the orthorhombic, space group P 2 1 2 1 2 1 , with a = 7.9476(6) Å, b = 11.6756(9) Å, c = 25.686(2) Å, α = β = γ = 90°, V = 2383.4(3) Å 3 , Z = 4. In this study, the pyridine at 1 , 2 were both involved in the classical ionic N–H⋯O H-bonds. The O–H⋯O H-bonds were also present in both salts. Apart from the classical H-bonds, the auxiliary interactions of CH⋯O, CH 3 –O, CH 3 –CH 3, CH–π, and O–π also helped the stabilization and expansion of the whole high-dimensional (3D) packings. Hirshfeld surface analysis provides additional views into the prevalence of the various short contacts in the crystal structure. On account of the subtle balance of the various nonbonding associations the synthons \(R_{2}^{2}\) (7), \(R_{2}^{2}\) (10), \(R_{3}^{2}\) (8), \(R_{3}^{2}\) (10), \(R_{3}^{3}\) (9), \(R_{3}^{3}\) (19), \(R_{4}^{3}\) (15), \(R_{4}^{4}\) (17), \(R_{5}^{4}\) (12) and \(R_{6}^{4}\) (18) were noted at the salts. For the combination of the classical H-bonds plus the various non-covalent contacts, the salts adopted the 3D net. In conclusion, we have shown that 3D structures can be constructed by the collective non-covalent interactions.
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Materials Horizons
·
2021
·Vol. 8
·期 12
·3432-3442
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IF 13.266
Fei Zhang,Xinzhen Ji,Wenqing Liang,Ying Li,Zhuangzhuang Ma,Meng Wang,Yue Wang,Di Wu,Xu Chen,Dongwen Yang,Xinjian Li,Chongxin Shan,Zhifeng Shi
Recently, the newly-emerging lead halide perovskite quantum dots (QDs) have attracted intensive research interest for lighting and display applications owing to their remarkable optoelectronic properties. It is regrettable that the toxicity and instability of lead largely hinder their practical applications. Here, zero-dimensional (0D) cesium indium halide (Cs3InX6) QDs were synthesized for the first time using a modified ligand-assisted reprecipitation method, and the emission wavelength can be tuned facilely via an anion exchange reaction. Typically, the Cs3InBr6 QDs showed broadband blue emission with a high photoluminescence (PL) quantum yield of 46%. First-principles calculations were performed and temperature-dependent PL was studied to investigate the emission mechanisms of the Cs3InBr6 QDs; the 0D nature of Cs3InBr6 enhances the localization of excitons, resulting in a large exciton binding energy. It is worth noting that the strong electron–phonon coupling of Cs3InBr6 indicates that the broadband emission comes from self-trapped exciton emission. Moreover, the Cs3InX6 QDs exhibit excellent stability against moisture, ultraviolet light and heat degradation, significantly better than for conventional lead halide perovskites. Subsequently, the white light-emitting diodes (WLEDs) prepared using blue-emissive Cs3InBr6 QD powder used as the phosphor showed an excellent working stability with a record half-life (T50) of 186 h. Even if the operating temperature is as high as 106.9 °C, the LED can still operate well and reach a T50 of 50 h. These results highlight the huge advantages and application potential of 0D Cs3InX6 QDs as an environmentally friendly emitter in the field of solid-state lighting.
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Bioresources and Bioprocessing
·
2018
·Vol. 5
·期 1
·1-11
·
IF 0
Liu Xin,Wang Weiwei,Hu Haiyang,Lu Xinyu,Zhang Lige,Xu Ping,Tang Hongzhi
Background Benzofuran and its derivatives contain central pharmacophores and are important structures in medicinal chemistry. Chemical synthesis of benzofuran rings often requires expensive catalysts and stringent operational conditions. Biosynthesis is recognized as a promising way to save energy and produce valuable compounds. Dioxin biodegradation pathways can form several benzofuran derivatives, and these pathways may be a better choice for further synthesis of important biological compounds. 2-Hydroxy-4-(3′-oxo-3′ H -benzofuran-2′-yliden)but-2-enoic acid (HOBB), a benzofuran derivative, can be biosynthesized from dibenzofuran (DBF) through co-metabolic degradation in a lateral dioxygenation pathway. Results Efficient biosynthesis of HOBB was observed using whole cells of Pseudomonas putida strain B6-2. After cultivation in LB medium containing biphenyl, the cells were suspended to an OD 600 of 5 to conduct biosynthesis in the presence of 0.5-mM DBF at pH 7 for 8 h. The bacterial cells were used twice to degrade approximately 0.70-mM DBF, and in batch process, accumulated about 0.29-mM HOBB. HOBB could be easily purified from the reaction with ethyl acetate using the neutral-acid extraction method, and 13.58 ± 0.31 mg of HOBB was obtained from 22.49 ± 0.74-mg DBF with an overall production yield of 60.4% (w/w). The product HOBB, which is a yellow powder, could be detected and identified by LC–MS, GC–MS, and NMR. Conclusions In this study, a new biological route was developed to produce HOBB from DBF using whole cells of P. putida B6-2 (DSM 28064). The biosynthesis of HOBB may contribute to studies of the DBF lateral pathway and provide a new green route for synthesizing benzofuran derivatives with pharmacological activities.
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Chemical Biology & Drug Design
·
2020
·Vol. 96
·期 6
·1433-1446
·
IF 2.548
Yibing Guo,Liancheng Xu,Changchun Ling,Tao Yang,Wenjie Zheng,Jin Lv,Qingsong Guo,Bohua Chen
Eighteen new β-carboline-based indole-4,7-quinone derivatives ( 12a–i and 13a–i ) were designed and synthesized, and their in vitro and in vivo antiproliferative activities were studied. Most of target compounds showed strong inhibition on three human tumor cells' proliferation. In particular, the most active compound 13g not only displayed more prominent antiproliferative activities than β-lapachone, a clinical antitumor candidate, but also exerted significant NAD(P)H: quinone-oxidoreductase-1 (NQO1) inhibitory activity and NQO1-dependent cytotoxicity in HT29 cells. Furthermore, 13g dose-dependently induced high ROS levels in HT29 cells, and selectively inhibited cancer cell but not non-tumor colon cell proliferation in vitro. Importantly, 13g promoted HT29 cell apoptosis and DNA damage by regulating relative apoptotic proteins and H2AX expression. Finally, 13g displayed significant growth inhibition of HT29 human colorectal adenocarcinoma xenograft in mice without overt toxicity.
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CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Haoquan Zhuang,Pengcheng Lin,Ying Chen
Janus evaporators achieve an energy utilization efficiency of 97.88%. • Janus evaporators demonstrate evaporation rates of 4.31 kg·m −2 ·h −1 . • Janus evaporators exhibit excellent long-term stability for 12 days. • Janus evaporators produce 18.53 kg·m −2 of fresh water per day. Solar interfacial evaporation is an emerging sustainable freshwater production technology. However, its effectiveness is often hindered by insufficient heat and mass transfer, the inherently high enthalpy of vaporization of water, and salt management issues. This study proposes a Janus-type photothermal semiconductor@biomass porous hydrogel evaporator to achieve high-rate and highly energy-efficient solar interfacial evaporation. Efficient biomass-based water transport channels were constructed through a microphase separation process and in-situ ionic crosslinking. The hydrophilic microenvironment of polar polymers was utilized to regulate the aggregation state of water molecules and reduce the equivalent enthalpy of vaporization. The Janus evaporator was assembled from photothermal semiconductors (tellurium nanoparticles) and biomass porous hydrogels to synergistically improve evaporation efficiency. Under one sun illumination, the evaporator achieved evaporation rates of 4.31 kg·m −2 ·h −1 in deionized water and 3.10 kg·m −2 ·h −1 in 3.5% simulated seawater, with an energy efficiency of 97.88%. Furthermore, due to the salt diffusion facilitated by the porous structure, it exhibited stable salt tolerance in simulated seawater with a high salinity of 10%. Outdoor natural seawater desalination experiments further confirmed its water production capacity and long-term stability, and the desalinated water quality met drinking water standards. This work provides a novel and forward-looking strategy for designing environmentally friendly, efficient, and stable solar evaporators.
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PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2020
·Vol. 22
·期 30
·17299-17305
·
IF 3.43
Chenyang Zhou,Ya Chu,Linlin Ma,Yingqian Zhong,Chao Wang,Yalan Liu,Haoyue Zhang,Beibei Wang,Xia Feng,Xi Yu,Xiaotao Zhang,Yan Sun,Xiaozeng Li,Guangjiu Zhao
In this work, we introduced halogen-substituted chiral molecules as A-site cations to synthesize a series of novel organic–inorganic hybrid two-dimensional (2D) chiral perovskite materials (R-X-p-mBZA)2PbBr4 (X = H, F, Cl, Br; p: para-position; mBZA = α-methylbenzylamine) for the first time. This halogen-substituted cation strategy collectively solved problems of narrow emission, weak chirality and low photoluminescence quantum yield (PLQY) for the emerged chiral perovskites. Photoluminescence (PL) spectra are significantly broadened due to the additional emission from self-trapped excitons (STEs) besides free excitons (FEs) states modulated by introducing significant disorder to the Pb–Br–Pb angle. The chirality of A-site chiral molecules is transferred and amplified to entire perovskite materials by fixing the chiral molecules at A-site via the interaction of halogen atoms. Furthermore, their PLQYs are improved with the reduction of energy gap and inhibition of the non-radiative transition from STEs to ground state. The halogen-substituted A-site cation strategy can be performed to develop organic–inorganic hybrid chiral perovskites with various optoelectronic applications.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Lei Wang,Hong Wang,Sinong Huang,Jiao Feng,Yifei Wu,Jing Deng,Junping Liu,Xiang Tu,Xiaoyan Ma,Xueyan Li,Andrea M. Dietrich
Complete dehalogenation of halogenated organic pollutants has attracted increasing attention, and electrocatalytic reduction processes are considered prospective technologies due to their high selectivity for carbon-halogen bonds. In this study, a vitamin B 12 (VB 12 ) composite electrode was prepared and applied to remove the refractory tribromoacetic acid (TBAA). The reduction process dominated by the VB 12 composite electrode showed a degradation efficiency of 55.2 % for 200 μg/L TBAA within 60 min. Interestingly, UV irradiation considerably increased the efficiency of TBAA for dehalogenation on the VB 12 composite electrode. The photoelectrochemical co-catalytic system of a VB 12 composite electrode coupled with UV (LP UV 254 nm) could remove 92.2 % of TBAA in 20 min with a rate constant 12 times higher than the VB 12 -only electrolysis system. The in situ Raman characterization and cyclic voltammetry tests confirmed that the accelerated formation of Co-Br bonds and the enhanced atomic H* mediated ability were responsible for improving debromination efficiency. The degradation of TBAA mainly underwent chemical reactions of debromination and mineralization. Acetic acid, formic acid, formaldehyde, and Br - were the major transformation products of TBAA. Acidic conditions favoured TBAA removal in the UV synergistic VB 12 electrolytic system, and excellent cycling stability of debromination was obtained in complex aqueous environments (actual bodies of water containing various inorganic and organic matter). This research provides an efficient dehalogenation technology for halogenated micropollutants and novel perspectives on the scientific design of photoelectrochemical dehalogenation processes.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Kuang Wang,Zhanqiang Fang
In this work, a cost-effective ball-milling technique was employed to synthesize submicron oxalated zero-valent iron co-doped with graphite and nickel (G@Fe OX bm /Ni), aiming to enhance the removal efficiency of the recalcitrant pollutant 2, 2′, 4, 4′ – tetrabromodiphenyl ether (BDE-47) while minimizing secondary risks. The incorporation of graphite significantly improved the debromination efficiency of BDE-47, with a rate constant of 0.26 day −1 in a tetrahydrofuran/water system, which represents a 59.88 % increase over the oxalated zerovalent Fe/Ni without graphite (0.16 day −1 ). The determination of Ni leaching showed that no nickel ions were detected post-reaction over a broad pH range (3–11). Moreover, the reactivity of G@Fe OX bm /Ni was largely unaffected across the pH range (0.26–0.49 day −1 ), exhibiting excellent resistance to acidic and alkaline conditions. In both ultrapure water and real groundwater matrices, the degradation rate constants for BDE-47 increased to 2.98 day −1 and 0.79 day −1 , respectively, achieving debromination yields of 97.86 % and 50.18 % for the final product, diphenyl ether. Based on the established degradation pathway and electrochemical analysis, the debromination of BDE-47 follows a catalytic debromination and hydrogenation process by adsorbed atomic hydrogen (H* ADS ). The graphite doping enhanced the debromination of BDE-47 by increasing the production of H* ADS . The adsorption effect of graphite on metal ions effectively controlled secondary pollution and improved the material’s tolerance to acidic and alkaline environments. This work offers an efficient method for the degradation of low brominated diphenyl ether pollutants at a low cost and without secondary risks.
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