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Solar RRL · 2021 ·Vol. 6 ·期 4 ·2100798 · IF 8.582

Controlling the Crystallographic Orientation of Sb2Se3 Film for Efficient Photoelectrochemical Water Splitting

Manjing Wang,Sanlong Wang,Qixing Zhang,Sanjiang Pan,Ying Zhao,Xiaodan Zhang

Finding a cost-effective semiconductor with commercial performance for photoelectrochemical (PEC) water splitting remains challenging. Sb 2 Se 3 , as a low-cost semiconductor, has excellent photo/electric properties for PEC water splitting. Via adjusting the Sb/Se ratio in the precursor ink, the Sb 2 Se 3 with favorable crystallographic orientation can be effectively controlled. The ink with an atomic ratio of Sb/Se = 1:3 induces the growth of a compact Sb 2 Se 3 film with a preferred orientation, resulting in rapid charge transport and high photocurrent. After depositing TiO 2 and Pt in turn, the photocathode with a structure of FTO/Au/Sb 2 Se 3 /TiO 2 /Pt exhibits a photocurrent density of 11.3 mA cm −2 at 0 V RHE . An unassisted solar water splitting device integrating the Sb 2 Se 3 -based photocathode with an inorganic perovskite photovoltaic cell achieves a solar-to-hydrogen efficiency of 2.45%. The efficient Sb 2 Se 3 -based photocathode shows promising potential for solar fuel production.

研究领域: 材料科学 · 物理化学 · 能源化学 · 半导体光电化学 · 可再生能源
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Advanced Materials Interfaces · 2018 ·Vol. 6 ·期 3 ·1801663 · IF 4.834

Ion Beam Defect Engineering on ReS2/Si Photocathode with Significantly Enhanced Hydrogen Evolution Reaction

Wentian Huang,Qingwei Zhou,Shaoqiang Su,Jing Li,Xubin Lu,Xingsen Gao,Xin Wang,Mingliang Jin,Guofu Zhou,Zhang Zhang,Junming Liu

Loading 2D layered transition metal dichalcogenides (TMDs) on p-type silicon photocathode is suitable for hydrogen production in solar-driven photoelectrochemical (PEC) water splitting. Similarly, various nanostructured TMDs exposing more active sites are widely explored for improving the PEC performances of composite photoelectrodes. Here, defect engineering using a controllable argon ion beam bombardment is presented on ReS 2 /Si photocathode. The atomic vacancy defects are introduced on the 2D ReS 2 to realize high-density active sites, which significantly enhance the solar-driven hydrogen evolution reaction performance of ReS 2 /Si photocathode. The highest photocurrent density of 18.5 mA cm −2 (at 0 V vs reversible hydrogen electrode) is achieved, under a simulated sun irradiation.

研究领域: 材料科学 · 光催化 · 能源化学 · 半导体器件 · 纳米科技
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Journal of Materials Chemistry A · 2014 ·Vol. 2 ·期 26 ·10169-10181 · IF 0

Development of supramolecular liquid-crystalline polyurethane complexes exhibiting triple-shape functionality using a one-step programming process

Shaojun Chen,Hongming Yuan,Shiguo Chen,Haipeng Yang,Zaochuan Ge,Haitao Zhuo,Jianhong Liu

Supramolecular liquid crystalline polymers and shape memory polymers are attracting increasing interest as materials. In this paper, we describe the development of a supramolecular liquid crystalline shape memory polyurethane (SLCSMPU) complex that exhibits both liquid crystalline properties and shape memory properties. The complex is formed by incorporating 4-hexadecyloxybenzoic acid (HOBA) into a pyridine-containing shape memory polyurethane (PySMPU). The HOBA is tethered to the PySMPU by strong hydrogen bonding between the pyridine rings and the COOH of the HOBA, forming a SLCSMPU complex. Heat treatment plays an important role in the formation of hydrogen-bonded supramolecular liquid crystalline structures in these SLCSMPU complexes. Thus, the SLCSMPU complex not only maintains the intrinsic liquid-crystalline properties of HOBA, but can also form a stable polymeric film for various shape memory applications. Additionally, the SLCSMPU complex forms a two-phase separated structure composed of an amorphous polyurethane matrix and a HOBA crystalline phase, which includes the hydrogen-bonded crystalline HOBA phase and the free HOBA crystalline phase. Therefore, a simple one-step programming process is developed that produces SLCSMPU complexes with excited triple-shape functionalities due to their multiple phase transitions, especially when the molar ratio of HOBA/BINA is less than 0.8.

研究领域: 高分子科学 · 材料化学 · 软物质物理 · 智能材料 · 功能高分子
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JOURNAL OF CATALYSIS · 2019 · IF 7.723

A switchable-selectivity multiple-interface Ni-WC hybrid catalyst for efficient nitroarene reduction

Yuanyuan Ma,Zhongling Lang,Jing Du,Likai Yan,Yonghui Wang,Huaqiao Tan,Shifa Ullah Khan,Yang Liu,Zhenhui Kang,Yangguang Li

Selective reduction of nitroarenes is extremely valuable in industrial chemical production. The main reduced products are usually aniline derivatives obtained using single-component noble- or transition-metal catalysts; however, other important products such as hydrazobenzene derivatives always involve in harsh conditions and multiple reaction steps. Here, we realize an unexpected switchable reduction of nitroarenes into aniline or hydrazobenzene derivatives with high yield and selectivity just by controlling the molar ratio of nitroarenes to N 2 H 4 ·H 2 O with a nickel–tungsten carbide composite nanocatalyst loaded on carbon (Ni-WC/C). A series of control experiments and density functional theory (DFT) calculations indicate that the multiple interfaces between Ni and WC can induce a synergistic effect, significantly modulating the electronic structure of the Ni-WC/C catalyst, and endowing the catalyst with switchable selectivity and high activity for the reduction of nitroarenes by hydrogenation. This synergistic multi-interfacial catalyst may offer a new way to design and explore highly efficient and selective catalysts for the controllable reduction of nitroarenes and similar hydrogenation reactions.

研究领域: 催化化学 · 有机合成 · 纳米材料 · 表面科学 · 工业化学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2022 · IF 9.965

Revealing the interfacial properties of halide ions for efficient and stable flexible perovskite solar cells

Zijun Yi,Bo Xiao,Xin Li,Yubo Luo,Qinghui Jiang,Junyou Yang

The severe non-radiative recombination loss caused by SnO 2 /perovskite interface defects greatly hinders the further improvement of the performance and stability of flexible perovskite solar cells (PSCs). Herein, a series of halides KM (M = F, Cl, Br, I) were inserted as interface layers to modulate the SnO 2 /perovskite interface. Both experimental and theoretical calculation demonstrated that F − exhibited stronger interface coupling effect between the SnO 2 and perovskite than other halide ions (Cl − , Br − , I − ). The F − had unique effects in effectively depressing SnO 2 /perovskite interface defects ascribed to the simultaneous formation of Sn F bonds and hydrogen bonds , resulting in reduced non-radiative recombination and improved interfacial contact. In consequence, the champion KF-modified flexible and rigid PSCs delivered outstanding PCE of 18.16 % and 21.36 %, accompanied by the enhanced V OC of 1.14 V and 1.16 V, respectively. Meanwhile, the stability of flexible PSCs was significantly ameliorated after KF modification, and about 84 % of the original efficiency could be retained even after 3000 bending cycles. This work provides a facile and efficient strategy for interface modulation to achieve high-performance and stable flexible PSCs.

研究领域: 材料科学 · 光伏技术 · 纳米界面工程 · 能源材料 · 半导体器件物理
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JOURNAL OF HAZARDOUS MATERIALS · 2021 · IF 10.588

Three porous shapeable three-component hydrogen-bonded covalent-organic aerogels as backfill materials in a simulated permeable reactive barrier (PRB) for trapping levofloxacin

Fangyuan Zhang,Mei Hong,Jing Bai,Zhi Liu,Aiyuan Jia,Zhisheng Liu,Can Shi,Yangxue Li

Levofloxacin (LEV) infiltrated in groundwater has threatened the safety of drinking water . For in-situ remediation of LEV-contaminated groundwater, there exists a main challenge of exploiting proper high efficient backfill medium in utilizing charming permeable reactive barriers (PRBs). Herein, three porous shapeable three-component hydrogen-bonded covalent organic aerogels (H C OA-1, H C OA-2 and H C OA-3) were fabricated based on a multiple-linking-site strategy to evaluate for adsorptive removal of LEV. The three H C OAs exhibited satisfactory performance in LEV adsorption that could integrate high adsorption capacity, good antiion interference, excellent recyclability and wide pH tolerance. The different regularity of kinetics and isotherms of three H C OAs signified that electrostatic effect, pore preservation, hydrogen bonding probably govern the adsorption process in combination, coupling with π-π electron-donor-acceptor (EDA), dipole-dipole and hydrophobic-hydrophobic interaction besides. In addition, the response surface methodology (RSM) was employed for studying the single and synergetic effects of selected variables and optimizing operation conditions. Furthermore, a laboratory PRB column packed with processable H C OA-2 was set up to investigate the LEV removal, and the breakthrough data was explained by Adams-Bohart, Thomas, BDST and Yoon-Nelson models. We believe could hopefully bring H C OAs into the real in-situ remediation of such challenging and persistent LEV-polluted groundwater with further massive-scale efficiently.

研究领域: 环境科学 · 材料科学 · 水污染控制 · 环境功能材料 · 污染物吸附 · 可持续修复技术
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Advanced Optical Materials · 2023 ·Vol. 11 ·期 22 ·2300888 · IF 9

Regulating Exciton Diffusion in Antimony-Based Perovskite-Like Single Crystals toward Highly Efficient and Stable Luminescence

Bihao Zhuang,Zicong Jin,Jiahuan Deng,Hui Xiong,Wenzhe Li,Jiandong Fan

Organic-inorganic hybrid metal halide perovskite has played an important role in optoelectronics and photonics due to their extremely high photoluminescence quantum yield (PLQY). However, considering the strong nonmetallic property of antimony (Sb), the excitons in antimony-based single crystals are usually dissipated in the form of non-radiative recombination under organic-inductive effect, which leads to the low PLQY. Herein, two kinds of perovskite-like single crystals, i.e., (8-HQ) 2 SbCl 3 and (8-HQH)SbCl 4 , are innovatively grown. The density functional theory (DFT) calculations reveal that the unique luminescence characteristics are associated with the inductive effect of organic coordination and exciton effect in the metal octahedral skeleton. When Cl − replaces the organic ligand in (8-HQ) 2 SbCl 3 , the inductive effect is reduced while the self-trapped exciton effect in the metal octahedron is enhanced. Besides, the theoretical research on electron transmission in a modeling device reveals that the hydrogen bond of organic A-site in the single crystal promotes the transition of electrons. Based on the luminescent properties of (8-HQH)SbCl 4 , the white LED devices are obtained by coating (8-HQH)SbCl 4 and red phosphor on 450 nm LED chips.

研究领域: 材料科学 · 光电子学 · 凝聚态物理 · 无机化学 · 半导体器件 · 光学材料 · 晶体工程
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Journal of Energy Storage · 2022 · IF 8.907

Facile synthesis and incomplete sulfidation of nickel-cobalt-aluminum ternary layered hydroxide binder-free electrode with enhanced supercapacitor properties

Kailin Li,Changqing Yin,Xingjian Dai,Jiayun Zhang,Shuang Yi,Jinsong Rao,Yuxin Zhang

Layered transition metal hydroxide, a clay-like material, possessing characteristics of large specific surface area, adjustable fraction, and plentiful active components make it a potential energy storage material , especially in the background of energy and environment crisis. Herein, comprehensive applications of cobalt-aluminum-based LDHs for supercapacitors are proposed. Binder-free electrodes were successfully synthesized such as Co 3 Al 1 -LDH/Ni, Ni 2 Co 1 Al 1 -LDH/Ni and Ni 1 Co 2 Al 1 -LDH/Ni using a rapid green hydrothermal approach. Subsequently, further sulfuration was carried out to obtain a heterostructure of sulfide/layered hydroxide. The electrochemical energy storage properties of binder-free electrodes were investigated, which show that the performance of ternary LDH electrode is better than that of binary one, and the incompletely sulfuration Ni 1 Co 2 S/Ni has the optimal electrochemical performance among all electrodes, with a specific capacitance of 2186 F g −1 at 1 A g −1 . The Ni 1 Co 2 S//AG hybrid supercapacitor (HSC) device assembled with Ni 1 Co 2 S as positive electrode and active graphene as negative electrode delivers an energy density of 13 Wh kg −1 at a power density of 749 W kg −1 , good rate capability and cycling stability.

研究领域: 材料科学 · 电化学 · 能源存储 · 纳米材料 · 功能材料 · 电化学储能
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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

One-step and sustainable preparations of inert additive-doped CaO-based CO2 adsorbents by hydrogenation reduction of CaCO3

Bao-Qi Feng,Han-Qing Chen,Chao Ping,Xiang Huang,Wen-Long Liu,Bao-Xia Dong,Yun-Lei Teng

The development of inert additive-doped CaO-based CO 2 adsorbents is a promising method to obtain efficient CO 2 adsorbents, while multiple programs are frequently involved, the organic solvent is often used, and CO 2 is sometimes released in the process of preparation. In this study, we first report that inert additive-doped CaO-based adsorbents can be synthesized in one pot by the mechanochemical hydrogenation reduction of CaCO 3 producing methane and avoiding CO 2 emission. The prepared CaO@C and CaO@MgO@C composites are high-performance CO 2 adsorbents with high CO 2 adsorption capacity and superior cycling stability. The results show that the CO 2 capture capacities of the CaO@C and CaO@MgO@C composites are 19.14 and 14.53 wt% higher than that of the BM-CaO (37.07 wt%), respectively, at 650 °C carbonation for 2 h. Notably, the activity losses of the CaO@C and CaO@MgO@C composites after 30 cycles are about 47.93 and 29.33%, which are much lower than that of the BM-CaO (60.39%). The performance of the CaO@C and CaO@MgO@C adsorbents is comparable to that of adsorbents synthesized by the conventional methods, but this work provides novel, simple, solution-free, and sustainable strategies to synthesize effective CaO-based CO 2 adsorbents in one pot.

研究领域: 材料科学 · 环境化学 · 能源工程 · 无机化学 · 碳捕集与封存 · 绿色化学 · 功能材料
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2021 · IF 5.816

Amine group ligand-modified hydrotalcite-like nano cobalt hydroxide for efficient oxygen evolution reaction

Jiali Gu,Xiaoli Yang,He Wang,Mengyuan Niu,Zhengyu Bai,Karthikeyan Kaliyappan,Lin Yang

The advancement of highly-efficient, non-noble metal electrocatalysts with high active sites for oxygen evolution reaction (OER) continues to face severe challenges. In this work, a new 3D flower-like α-Co(OH) 2 catalyst with high Co–NH 2 active sites (referred to as α-Co(OH) 2 –NH 2 ) is prepared. The Co–NH 2 active sites are formed through the interactions between Co 2+ and –NH 2 groups and exhibit higher electrocatalytic performance for OER in alkaline mediums, with a lower overpotential (300 mV at 10 mA cm −2 ), a flatter Tafel slope (75 mV dec −1 ) and a longer stability. Moreover, water splitting catalyzed by α-Co(OH) 2 –NH 2 delivers 1.62 V to reach a current density of 10 mA cm −2 . The mechanism studies show that the OER electrocatalytic activity is closely related to the content of –NH 2 . Density functional theory (DFT) calculations unveil that –NH 2 groups can facilitate the formation of OH∗ on the α-Co(OH) 2 surface and promote the desorption of O 2 ∗ into O 2(g) .

研究领域: 材料化学 · 电化学 · 纳米催化 · 能源材料 · 计算化学
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Science China-Materials · 2020 ·Vol. 63 ·期 7 ·1182-1195 · IF 6.098

Ultrasmall NiFe layered double hydroxide strongly coupled on atomically dispersed FeCo-NC nanoflowers as efficient bifunctional catalyst for rechargeable Zn-air battery

Wang Yiyan,Zhang Guoxin,Ma Mang,Ma Yan,Huang Jiankun,Chen Chen,Zhang Ying,Sun Xiaoming,Yan Zifeng

An atomically dispersed FeCo-NC material with the 3D flower-like morphology was used as a unique substrate for the controllable deposition of ultrasmall NiFe layered double hydroxide nanodots (termed as NiFe-NDs) to simultaneously promote the sluggish kinetics of oxygen reduction reaction (ORR) and oxygen evolution reaction (OER). The size-limiting growth of NiFe-NDs (~4.0 nm in diameter) was realized via the confinement of the 3D flower-like mesoporous structure and the rich N/O functionality of FeCo-NC. Benefiting from the distinctive structure with the simultaneously maximum exposure of both OER and ORR active sites, the NiFe-ND/FeCo-NC composite showed an ORR halfwave potential of 0.85 V and an OER potential of 1.66 V in 0.1 mol L −1 KOH at 10.0 mA cm −2 . In-situ Raman analysis suggested the activity of OER was derived from the Ni sites on NiFe-ND/FeCo-NC. Moreover, the NiFe-ND/FeCo-NC-assembled Zn-air battery (ZAB) exhibited a very small discharge- charge voltage gap of 0.87 V at 20 mA cm −2 and robust cycling stability. Furthermore, the NiFe-ND/FeCo-NC composite was also applicable for fabricating all-solid-state ZAB to power wearable electronics with superior cycling stability under deformation. Our work could enlighten a new applicable branch of atomically dispersed metal-nitrogen-carbon materials as unique substrates for fabricating multifunctional electrocatalysts.

研究领域: 材料科学 · 电化学 · 能源存储 · 催化化学 · 纳米科技
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NEW JOURNAL OF CHEMISTRY · 2022 ·Vol. 46 ·期 6 ·2837-2845 · IF 3.925

Organic spacer engineering in 2D/3D hybrid perovskites for efficient and stable solar cells

Xiaofang Ye,Hongkun Cai,Qinghe Sun,Tie Xu,Jian Ni,Juan Li,Jianjun Zhang

Perovskite solar cells (PSCs) have attracted widespread attention owing to their adjustable band gap, easy manufacturing, and longer carrier diffusion length. However, the influence of environmental factors such as water, oxygen, light and heat, as well as the inherent ionic characteristic of the perovskite crystal, make the stability of the device relatively poor. Here, organic cation ammonium salts, due to their hydrophobicity, are used as the 2D/3D hybrid perovskite isolation layer, and the spacer cation and inorganic [PbI6]4− octahedral structure could form multiple NH⋯I hydrogen bonds, which make the devices not only have the excellent long-term stability of 2D perovskites but also the high efficiency of 3D perovskites. At the same time, the EDS mapping results prove that ion migration and diffusion are significantly suppressed. As a result, in comparison with the control device (PCE = 19.41%), the PCE of the solar cell with a 2D capping layer based on PMAI is slightly increased to 20.02%, and the stability still maintains 93.02% of the original efficiency after 720 hours. In addition, both the long alkyl chain and the benzene ring can improve the hydrophobicity of the film, while the benzene ring can better enhance the humidity stability. This work provides a guide for developing 2D/3D PSCs to balance high efficiency and good long-term stability.

研究领域: 材料科学 · 光伏技术 · 纳米结构材料 · 能源化学 · 半导体器件
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