Journal of Energy Chemistry
·
2022
·
IF 13.599
Yang Ding,Soumyajit Maitra,Chunhua Wang,Runtian Zheng,Meiyu Zhang,Tarek Barakat,Subhasis Roy,Jing Liu,Yu Li,Tawfique Hasan,Bao-Lian Su
Graphitic carbon nitride (g-C 3 N 4 ) has attracted great interest in photocatalysis and photoelectrocatalysis. However, their poor hydrophilicity poses a great challenge for their applications in aqueous environment . Here, we demonstrate synthesis of a hydrophilic bi-functional hierarchical architecture by the assembly of B-doped g-C 3 N 4 nanoplatelets . Such hierarchical B-doped g-C 3 N 4 material enables full utilization of their highly enhanced visible light absorption and photogenerated carrier separation in aqueous medium , leading to an excellent photocatalytic H 2 O 2 production rate of 4240.3 μM g −1 h −1 , 2.84, 2.64 and 2.13 times higher than that of the bulk g-C 3 N 4 , g-C 3 N 4 nanoplatelets and bulk B doped g-C 3 N 4 , respectively. Photoanodes based on these hierarchical architectures can generate an unprecedented photocurrent density of 1.72 mA cm −2 at 1.23 V under AM 1.5 G illumination for photoelectrochemical water splitting. This work makes a fundamental improvement towards large-scale exploitation of highly active, hydrophilic and stable metal-free g-C 3 N 4 photocatalysts for various practical applications.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2018
·
IF 11.698
Shuai Zhao,Zan Dai,Wenjin Guo,Fengxi Chen,Yunling Liu,Rong Chen
Selective oxidation of glycerol to produce aimed high-value added products is of great importance in chemical industry. Photocatalytic oxidation provides a promising and green strategy for selective glycerol oxidation. In this work, we develop a Bi/Bi 3.64 Mo 0.36 O 6.55 heterostructure via a facile solvothermal method for the selective oxidation glycerol to 1, 3-dihydroxyacetone (DHA) in water under visible light irradiation. The excellent performance in activity and selectivity of Bi/Bi 3.64 Mo 0.36 O 6.55 heterostructure for DHA production is attributed to a dual-pathway photocatalytic reaction process. The mass production 1 O 2 ascribed to the reduced energy gap (ΔE ST ), the enhanced spin-orbit coupling (SOC) and the presence of oxygen vacancy is beneficial for the selective oxidation of glycerol to DHA. Simultaneously, the metallic bismuth in the heterostructure promotes the separation of photogenerated holes with efficient redox potential and facilitates the binding bismuth with ortho-hydroxyl in glycerol, thus enhancing the yield and selectivity of DHA production. This work provides a novel strategy and thorough understanding of the development of highly efficient bismuth-based photocatalyst for selective oxidation in organic reactions.
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Materials Today Physics
·
2022
·
IF 11.021
Shibo Wang,Fengxian Cao,Weihai Sun,Chunyan Wang,Zhongliang Yan,Nan Wang,Zhang Lan,Jihuai Wu
All-brominated inorganic perovskite CsPbBr 3 has received much attention in the field of optoelectronic applications owing to its superb stability and ease of manufacture under the ambient condition. However, the tedious process and toxic solvent are two major challenges for fabrication of CsPbBr 3 films via a multi-step deposition method . Here, we demonstrate a sustainable bi-solvent system for preparing high-quality CsPbBr 3 films in a triple-step solution-processed route, where the bi-solvent system comprises of green solvent water and ethylene glycol monomethyl ether (EGME) in place of the noxious methanol for CsBr solution. By adjusting the temperature of heat treatment and spin-coating speed, the pinhole-free, ultra-smooth and high crystallinity of CsPbBr 3 films were obtained. As a result, the CsPbBr 3 PSC prepared from the green bi-solvent system demonstrates an optimal power conversion efficiency (PCE) of 9.55%, which is one of the highest efficiencies for planar carbon-based PSCs without hole transport layer. Moreover, the all-inorganic unpacked PSCs exhibit excellent humidity stability under ambient environment for 34 days. Our result not only offers a facile and simple way to fabricate the pure-phase CsPbBr 3 films, but also alleviates the solvent toxicity during the preparation of CsPbBr 3 PSCs.
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Reaction Kinetics Mechanisms and Catalysis
·
2024
·
IF 1.7
Lin Guangqiang,Mao Chunfeng,Li Menghua,Wang Ziyi,Li Qinyi,Zhan Jiaqing,Liu Junsheng
In this study, Zn–W–Bi–O catalysts with a sandwich structure were prepared by mixing zinc tungstate and bismuth nitrate to form bismuth tungstate at the interface. The catalyst was composed of bismuth nitrate as the upper layer, zinc tungstate as the lower layer, and phase interface (bismuth tungstate) as the core. The generation of phase interfaces provides a new reaction mechanism for catalytic processes. Based on the different intermediate state changes in the reaction process, the Zn–W–Bi–O catalysis system can be divided into H-S Mechanism, B-R Mechanism, and P-G Mechanism. These reaction mechanisms will simultaneously react with H 2 O 2 to generate various transition states, which will cooperatively oxidize sulfur atoms to remove them. The structural characteristics and stability of Zn–W–Bi–O catalysts were determined. There are strong stability and catalytic efficiency for Zn–W–Bi–O catalysts. The desulfurization rate can be close to 100% under optimal conditions (Catalyst of 0.02 g, ionic liquids of 0.5 mL, H 2 O 2 of 0.2 mL, model oil of 5 mL, 80 °C). Zn-W-Bi-O-2 catalysts lead to 3 times improvement in ODS activity for the upper layer and 1.25 times improvement in ODS activity for the lower layer. The catalytic reaction mechanism was obtained by the structure-activity relationship.
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Molecular Catalysis
·
2024
·
IF 3.9
Liwen Yin,Qianqian Zhang,Hefeng Cheng,Yuanyuan Liu,Baibiao Huang,Peng Wang
Photocatalytic synthesis of carbonyl compounds (aldehydes or ketones) offers great potential for sustained development in the production of pharmaceuticals and fine chemicals. Nevertheless, exploring photocatalysts with high stability, activity, and selectivity remains a significant challenge. In this study, Cs 3 Bi 2 Br 9 (CBB) perovskite nanocrystals have been successfully fabricated by confining the in-situ growth of perovskite CBB within mesoporous molecular sieve SBA-3. The obtained nanocrystals (2–4 nm) possess the advantages of excellent stability, exceptional dispersibility, abundant active sites, and enhanced charge carrier separation capability. Under visible light irradiation and air atmosphere, the CBB@SBA-3 could effectively oxidize benzyl alcohol to benzaldehyde with a total yield of 98.9 μmol, which is 22 times superior to that of bulk CBB, accompanied by a remarkable 99 % selectivity. Comparative experiments and in situ characterizations reveal the roles of electron ( e − ), hole ( h + ), and superoxide radical (·O 2 − ), while successfully capturing the carbon intermediates (·C) during the reaction process, further providing a comprehensive elucidation of the mechanism underlying the conversion of benzyl alcohol to benzaldehyde. This work is expected to provide insights into extending the design and photocatalytic application of Bi-based halide perovskite nanocrystals.
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ACS Catalysis
·
2025
·
IF 13.1
Lecheng Liang,Hengyu Li,Peng Li,Jinhui Liang,Shao Ye,Binwen Zeng,Mingjia Lu,Yanhong Xie,Yucheng Wang,Taisuke Ozaki,Shengli Chen,Zhiming Cui
A long-standing puzzle for methanol electrooxidation is the fundamental understanding of the origin of electrocatalytic selectivity. Herein, we unequivocally demonstrate that the Bi-modified Pt/C follows a CO-free dominated pathway during alkaline methanol electrooxidation and unveil the formaldehyde (HCHO) intermediate as a critical factor influencing pathway selectivity. These findings are substantiated by kinetic isotope effects, formate Faradaic efficiency, in situ spectroscopy, ab initio molecular dynamics simulations, and density functional theory calculations. Bi modification significantly increases the HCHO dehydrogenation barrier, which facilitates its desorption and subsequent conversion to the H2COOH– anion at the alkaline interface, intrinsically avoiding CO formation. More specifically, the formation of ensemble sites featuring a V-shaped Bi–Pt–Bi configuration inhibits the cleavage of the C–H bond, and the weak OH binding energy at Bi adatoms effectively prevents blockage of oxygenated species, allowing such ensemble sites to fulfill their functional role. This work provides in-depth insights into the origins of pathway selectivity and benefits the theory-guided design of advanced CO-free electrocatalysts.
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ADVANCED FUNCTIONAL MATERIALS
·
2023
·Vol. 33
·期 22
·2300582
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IF 19
Ziquan Li,Jinquan Wen,Yuqing Cai,Fengting Lv,Xu Zeng,Qian Liu,Titus Masese,Chuanxiang Zhang,Xusheng Yang,Yanwen Ma,Haijiao Zhang,Zhen-Dong Huang
Potassium-ion batteries have emerged not only as low-cost alternatives to lithium-ion batteries, but also as high-voltage energy storage systems. However, their development is still encumbered by the scarcity of high-performance electrode materials that can endure successive potassium-ion uptake. Herein, a hydrated Bi-Ti bimetallic ethylene glycol (H-Bi-Ti-EG) compound is reported as a new high-capacity and stable anode material for potassium storage. H-Bi-Ti-EG possesses a long-range disordered layered framework, which helps to facilitate electrolyte ingress into the entire Bi nanoparticles. A suite of spectroscopic analyses reveals the in situ formation Bi nanoparticles within the organic polymer matrix, which can alleviate stresses caused by the huge volume expansion/contraction during deep cycles, thereby maintaining the superior structural integrity of H-Bi-Ti-EG organic anode. As expected, H-Bi-Ti-EG anode exhibits a high capacity and superior long-term cycling stability. Importantly for potassium storage, it can be cycled at current densities of 0.1, 0.5, 1, and 2 Ag −1 for 800, 700, 1000, and even 6000 cycles, retaining charging capacities of 361, 206, 185, and 85.8 mAh g −1 , respectively. The scalable synthetic method along with the outstanding electrochemical performance of hydrated Bi-Ti-EG, which is superior to other reported Bi-based anode materials, places it as a promising anode material for high-performance potassium storage.
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MATERIALS RESEARCH BULLETIN
·
2025
·
IF 5.7
Juan Liu,Yingnan Qin,Meiqi Wang,Hengjun Liu,Tao Zheng,Jing Tian,Jing Wang
BiVO 4 -based materials have attracted extensive research as advanced photoanode for photogenerated cathodic protection. However, the performance of BiVO 4 -based photoanodes is greatly hindered by its weak charge migration and positive conduction band potential. Herein, poly-2,6-diaminoanthraquinone (PDAAQ)/Bi was grafted on BiVO 4 to improve the separation efficiency of photogenerated carriers and enhance the reducing ability of photogenerated electrons. Studies show that a type II heterojunction can be formed between PDAAQ and BiVO 4 , which accelerates the separation of photogenerated carriers at the interface. In addition, the Bi monomers anchored on BiVO 4 /PDAAQ then expand the light absorption range through the surface plasmon resonance effect. Consequently, the obtained BiVO 4 /PDAAQ/Bi photoanode exhibits a promising photocurrent density of 40 μA·cm -2 , while the photoinduced potential drop is 540 mV, which is approximately 1.4 times of BiVO 4 materials. These outcomes provide general ideas for the design of organic-inorganic heterozygous systems for achieving eco-friendly corrosion protection.
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Nano-Micro Letters
·
2025
·Vol. 17
·期 1
·1-16
·
IF 36.3
Liu Xiaoji,Duan Yuping,Wu Nan,Li Guangming,Guo Yuan,Liu Jiangyong,Zhu Ning,Wang Qiang,Wang Lin,Xu Zichen,Wei Hao,Wang Guojun,Zhang Zhijia,Zhang Songsong,Zhou Wenjun,Ma Teng,Wang Tongmin
Magnetic absorbers with high permeability have significant advantages in low-frequency and broadband electromagnetic wave (EMW) absorption. However, the insufficient magnetic loss and inherent high conductivity of existing magnetic absorbers limit the further expansion of EMW absorption bandwidth. Herein, the spinel (FeCoNiCrCu) 3 O 4 high-entropy oxides (HEO) are successfully constructed on the surface of FeCoNiCr 0.4 Cu 0.2 high-entropy alloys (HEA) through low-temperature oxygen bath treatment. On the one hand, HEO and HEA have different magnetocrystalline anisotropies, which is conducive to achieving continuous natural resonance to improve magnetic loss. On the other hand, HEO with low conductivity can serve as an impedance matching layer, achieving magneto-electric co-modulation. When the thickness is 5 mm, the minimum reflection loss (RL) value and absorption bandwidth (RL < − 5 dB) of bi-phase high-entropy composites (BPHEC) can reach − 12.8 dB and 633 MHz, respectively. The RCS reduction value of multilayer sample with impedance gradient characteristic can reach 18.34 dB m 2 . In addition, the BPHEC also exhibits temperature-stable EMW absorption performance, high Curie temperature, and oxidation resistance. The absorption bandwidth maintains between 593 and 691 MHz from − 50 to 150 °C. This work offers a new and tunable strategy toward modulating the electromagnetic genes for temperature-stable ultra-broadband megahertz EMW absorption.
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Journal of Energy Storage
·
2024
·
IF 8.9
Yaqing Wang,Qiujun Wang,Di Zhang,Zhaojin Li,Huilan Sun,Qujiang Sun,Bo Wang
Solid-state lithium metal batteries (SSLMBs) are considered to be the next generation of high safety and high energy density storage device. However, the accidental lithium dendrites growth and the solid-solid contact problem have seriously hindered the development of their commercialization. Therefore, it is of great significance to develop high-modulus electrolytes to suppress lithium dendrites growth and achieve close-knit contact between electrolyte/electrodes. Herein, we utilize the natural settlement of Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 (LLZTO) during in-situ polymerization method of polyester-based trimethylolpropane trimethacrylate (TMPTMA) and 1,6-hexanediol diacrylate (HDDA) monomer and the based on the selective adsorption of glass fiber to construct an asymmetric bi-functional composite electrolyte membrane (A-P(PF) 1 TH-X%LLZTO). To match the high voltage cathode material, the polymer electrolyte matrix containing ploy (vinyl carbonate) (PVC)/lithium difluoro(oxalato) borate (LiDFOB) was introduced into the pore of the cathode material to construct stable cathode electrolyte interphase (CEI) layer on the surface of the active material. The characterization of Li solid NMR spectra shows that the ceramic oxides provide effective pathways for the Li + conduction between the asymmetric electrolyte and the lithium anode. Symmetric Li Li cells exhibit low charge voltage polarization, can operate stably at 0.2 mA cm −2 for over 700 h, and can increase the critical current density to 2.1 mA cm −2 . The lithium metal batteries (LMBs) assembled with high voltage LiCoO 2 cathode has the capacity retention rate of 99.62 % after 500 cycles (remained 118.08 mAh g −1 at 1C). Such excellent electrochemical properties are attributed to the establishment of asymmetric electrolytes that can form inorganic component-rich SEI layer on the side of Li metal. This work demonstrates an effective interface engineering strategy that can simultaneously realize the interface stability of the cathode and anode electrode/solid electrolyte, which shows great potential for promoting the development of LMBs.
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ACS Catalysis
·
2026
·Vol. 16
·期 15
·14804-14817
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IF 13.6
Liu Hongjing,Ren Shan,Li Xiaodi,Liu Manyi,Chen Peng,He Chi,Bai Bofeng,Chai Shouning,Dong Fan
Efficient photocatalytic mitigation of nitrogen oxides (NO x ) under ambient conditions remains challenging due to limited charge-carrier separation and poor selectivity in regulating reactive oxygen species (ROS), which often results in undesirable NO 2 accumulation. In this study, bismuth molybdate (Bi 2 MoO 6 ) was employed as a model photocatalyst, on which dual active sites composed of plasmonic metallic Bi nanoparticles and ultrasmall spin-polarized NiO were in situ constructed. Plasmonic Bi enhances visible-light absorption and hot-electron generation via localized surface plasmon resonance, while NiO establishes a spin-selective electron-transfer pathway that facilitates efficient O 2 activation. This cooperative interface suppresses exciton recombination and promotes a superoxide (·O 2 – )-dominated oxidation pathway. Consequently, the optimized Bi-NiO@BMO achieves 77.0% NO removal, 76.7% nitrate selectivity, and minimal NO 2 accumulation (<11 ppb), representing a 9.7-fold enhancement compared with pristine Bi 2 MoO 6 . In practical applications, the PTFE-assisted loading technique allows the material to be fixed onto ceramic foam, achieving an 84% NO removal efficiency and further enhancing photocatalytic performance. Spectroscopic analyses combined with density functional theory (DFT) calculations confirm that the plasmon–spin interaction lowers the free-energy barriers for ·O 2 – formation and deep NO oxidation. This work provides a mechanistic insight into plasmon-spin-regulated ROS generation and offers a rational design strategy of highly selective photocatalysts for environmental NO x abatement.
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Nature Communications
·
2026
·Vol. 17
·期 1
·1699
·
IF 15.7
Sui Huiting,Lou Wenhua,Xiao Shibing,He Jia,Wu Fuling,Liu Ying,Wei Jianbiao,Lu Haijie,Sun Huajun,Ma Xiaoguang,Zhang Shujun
Defect microstructures, particularly dislocations, are pivotal in determining the functional properties of ferroelectric thin films. While their density is routinely considered, the critical role of their spatial configuration has remained largely unexplored and difficult to control. Here, we develop a controlled self-assembly strategy for dislocations in Bi(Fe,Mn)O 3 thin films on Ni-Cr that directly addresses this challenge. By employing a LaNiO 3 buffer layer, we template a discontinuous-columnar grain structure and guide the self-assembly of edge dislocations along grain boundaries in a topologically-protected configuration. The resulting ordered microstructure promotes a more uniform strain field and more coherent FeO 6 octahedral tilting, significantly enhances polarization homogeneity, leading to a lower domain-switching barrier and a more uniform domain pinning effect. Consequently, the BFMO thin film exhibits dramatically superior aging stability after 60 days at 60 °C, exhibiting far smaller reductions in remanent polarization (~20%) and coercive field (~35%) compared to the BFMO thin film grown directly on Ni-Cr. These findings establish a defect engineering paradigm wherein the deliberate dislocation rearrangement is leveraged to unlock superior ferroelectric performance.
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