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Science China Chemistry 2025年

作者： Rui Yu Xi Cao Chengyang Zhu Qingqing Chen Ziyi Yan Binbin Jiang Junjie Mao Xianwen Wei key laboratory of Electrochemical clean energy of Anhui Higher Education Institutes College of Chemistry and Materials ScienceAnhui Normal University Anhui provincial key laboratory of Advanced Catalysis and energy Materials School of Chemistry and Chemical Engineering Anqing Normal University School of Chemistry and chemical Engineering Anhui University of Technology

Developing highly efficient and cost-effective electrocatalysts for hydrogen evolution reaction（HER） is grandly challenging in alkaline and alkaline seawater electrolytes. Herein, the asymmetric interfacial active sites with Ru nanoparticles and Ni single atoms in Ru/Ni-N-C were designed through a solvothermal-pyrolysis process. Constructing highly asymmetric interfacial active sites with a strong electron delocalization effect significantly improves HER kinetics. As expected, Ru/Ni-N-C requires low overpotentials with around 20 mV at 10 mA cm-2and robust durability over 48 h in alkaline and alkaline seawater *** at 200 mA cm-2, the overpotentials are close to 100 mV in both above electrolytes for Ru/Ni-N-C. Density function theory calculation results suggest that the asymmetric interface between Ru nanoparticle and Ni-N-C could accelerate the dissociation of water molecules and modulate the hydrogen species, consequently improving the HER performances. This work opens a unique approach for constructing advanced materials for energy conversion.

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Insights into spin polarization regulated exciton dissociation and charge separation of C_(3)N_(4)for efficient hydrogen evolution and simultaneous benzylamine oxidation

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Nano Research 2023年第7期16卷 8845-8852页

作者： Gen Li Xiaomei Sun Peng Chen Meiyang Song Tianxiang Zhao Fei Liu Shuang-Feng Yin provincial guizhou key laboratory of green chemical and clean energy technology School of Chemistry and Chemical EngineeringGuizhou UniversityGuiyang 550025China College of Chemistry and chemical Engineering Advanced Catalytic Engineering Research Center of the Ministry of EducationState Key Laboratory of Chemo/Biosensing and ChemometricsHunan UniversityChangsha 410082China

The employment of spin polarization under an external magnetic field holds great potential for the improvements of photocatalytic ***,owing to the huge difference in dielectric properties between ferromagnetic oxide and polymers,the photogenerated excitons with spin states are often limited to the ferromagnetic oxide wells,which leads to unsatisfactory *** this paper,a single-atom Co-doped C_(3)N_(4)photocatalyst is successfully synthesized for photocatalytic water splitting and simultaneous oxidation of *** a tiny external magnetic field(24.5 mT),the hydrogen production rate could reach at 3979.0μmol·g^(-1)·h^(-1),which is about 340 times that of C_(3)N_(4).Experimental results and theoretical calculations indicate that the interaction of Co d and N p orbital changes the symmetry center of C_(3)N_(4),resulting in an increase in dielectric constant and spin ***,magnetic fields further promote parallel electron spin,and the increased number of charges with the parallel spin-down state is likely to dissociate under the action of an external magnetic *** the other hand,the Co-N bond provides a huge built-in electric field and active site for strengthening the charge transfer and surface *** work not only deepens the understanding of spin polarization,but also enriches methods to accelerate electron-hole separation.

关键词： low magnetic field C_(3)N_(4) spin polarization photocatalytic hydrogen evolution benzylamine oxidation

Enhancing the hydration reactivity of hemi-hydrate phosphogypsum through a morphology-controlled preparation technology

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Chinese Journal of chemical Engineering 2016年第9期24卷 1298-1305页

作者： Lin Yang Jianxin Cao Caiyu Li School of Chemistry and chemical Engineering Guizhou UniversityGuiyang 550025China College of Resource and Environmental Engineering Guizhou UniversityGuiyang 550025China guizhou key laboratory.for green chemical and clean energy technology Guiyang 550025China

The distribution of water channels in the crystal morphology of type-α hemi-hydrated gypsum(α-HH) was theoretically detected to investigate the effect of water channels on the hydration reactivity of hemi-hydrate phosphogypsum(HPG). Results showed that water channels were mainly distributed in the cylinders of α-HH crystal,whereas no water channel existed in the conical surfaces parallel to the z-axis. Increasing the number of water channels was critical to enhance the hydration activity of HPG compared with the hydration reactivity of industrial HPG and type-α high-strength gypsum. Controlling the technological parameters of crystallization by concentration of liquid-phase SO_4^(2-) made it possible to obtain HPG which had the stumpy crystals of α-HH and high hydration reactivity.

关键词： Hydration reactivity Morphology-controlled Water channel Hemi-hydrated phosphogypsum

The effect of copper valence on catalytic combustion of styrene over the copper based catalysts in the absence and presence of water vapor

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Chinese Journal of chemical Engineering 2016年第4期24卷 468-474页

作者： Hongyan Pan Zhiyan He Qian Lin Fei Liu Zhong Li School of chemical Engineering Guizhou University Cuiyang 550025 China key laboratory of guizhou Province for green chemical Industry and clean energy technology Guiyang 550025 China Research Institute of chemical Engineering South China University of Technology Guangzhou 510640 China

Catalysts CuOx/γ,-Al2O3-IH and CuOx/γ/-Al2O3-IM were prepared, characterized, and tested for styrene combustion in the absence and presence of water vapor. The effect of copper valence of the catalysts on the catalytic activity for styrene combustion was discussed using the theory of hard soft acids and bases （HSAB）. The results showed that the existence of water vapor in feed stream inhibited the catalytic activity for styrene combustion due to the competition adsorption of water molecule. HSAB theory confirmed that the local soft acidity of the catalyst CuOx/^-AI203-1H was much stronger than that of the catalyst CuOx/^-AI203-1M because of the higher content of soft acid Cu＋ on its surface, which increased the adsorption ability toward soft base of styrene and reduced the adsorption toward hard base of water vapor, and thus increased the catalytic activity for styrene combustion and weakened the negative influence of water vapor.

关键词： Catalyst combustionStyreneCopper based catalystsWater inhibitionTheow of hard soft acids and bases

Effect of CeO_(2)on Activity of Catalysts CuO/ZnO/Al_(2)O_(3)/CeO_(2)for Synthesis of Methanol

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China Petroleum Processing & Petrochemical technology 2023年第3期25卷 104-114页

作者： Zhou Songhua Li Wenbo Wu Zongjin Chen Zhongyang Huang Chen Zhang Chuanwei Wang Bo Pan Hongyan Lin Qian 无 guizhou Tianfu chemical Industry Co. LtdFuquan550501China Department of chemical Engineering School of Chemistry and Chemical EngineeringGuizhou UniversityGuiyang 550025China guizhou key laboratory for green chemical and clean energy technology Guiyang 550025China

The size of the nanoparticles and the number of oxygen vacancies have a significant effect on the catalytic activity of copper-based catalysts used for the synthesis of methanol from *** this study,the authors prepared a series of catalysts CuO/ZnO/Al_(2)O_(3)/CeO_(2)(CZAC)with CuO particles of different sizes and varying number of oxygen vacancies on the surface by changing the added volume of CeO2 by using the co-precipitation *** properties of the catalysts were characterized and their activity was evaluated by using high-pressure fixed-bed reaction *** results showed that the addition of CeO_(2)to CuO/ZnO/Al_(2)O_(3)not only influenced the size of the CuO particles and metal-metal interactions,but also had an effect on the concentrations of oxygen vacancies and strongly basic *** presence of CuO particles of small sizes and a large numbers of oxygen vacancies on the surface of the catalyst were beneficial to its activity for the synthesis of *** catalyst CZAC,when modified by 5%of CeO_(2),recorded CuO particles of the smallest size(8.9 nm),strong intermetallic interactions,and the highest concentrations of oxygen vacancies and strongly basic *** also exhibited the highest catalytic activity,with a space-time yield of methanol of 0.315 g/(h·g)that was higher than that of the enterprise RK-5 catalyst[0.215 g/(h·g)].

关键词： catalyst amount of CeO_(2)added size of CuO particles oxygen vacancies methanol synthesis

Insights into the synergistic promotion of spin polarization over C_(3)N_(5.4) for enhancing cooperative hydrogen evolution and benzylamine oxidation coupling

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Nano Research 2023年第4期16卷 4225-4232页

作者： Qiuchen Wang Xiaoxu Deng Haiyan Pen Fei Liu Meiyang Song Peng Chen Shuang-Feng Yin provincial guizhou key laboratory of green chemical and clean energy technology School of Chemistry and Chemical EngineeringGuizhou UniversityGuiyang 550025China College of Big Data and Information Engineering Guizhou UniversityGuiyang 550025China College of Chemistry and chemical Engineering Advanced Catalytic Engineering Research Center of the Ministry of EducationState Key Laboratory of Chemo/Biosensing and ChemometricsHunan UniversityChangsha 410082China

Polymers are usually restricted on the high exciton binding energies and sluggish electron transfer because of the low dielectric *** spin-polarized electrons is regarded as an attractive strategy,but often confined to the d-orbital ***,the nonmetal P and N elements co-mediated the spin polarization of carbon nitrides(PCN)have been elaborately *** optimized PCN-3 shows an outstanding hydrogen production(22.2 mmol·g^(-1)·h^(-1))coupled with selective benzylamine oxidation without using any solvent and cocatalysts,which is 200 times of original C_(3)N_(4)and superior to the photocatalysts has been reported to *** and theoretical results verified that the spin-orbital coupling of N 2p and P 2p remarkably increased the parallel spin states of charge and reduced the formation of singlet excitons to accelerate exciton dissociation in carbon *** addition,charge separation and surface catalysis can be significantly enhanced by the electron spin polarization of carbon nitride with the parallel arrangement,huge built-in electric field and disturbed electronic *** finding deepens the insight into the charge separation and exciton dissociation in spin polarization,and offers new tactics to develop high-efficiency catalysts.

关键词： spin polarization photocatalysis amine oxidative coupling hydrogen production C_(3)N_(5.4)

Deep decalcification of factory-provided freezing acidolysis solution to achieveα-high-strength gypsum

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Chinese Journal of chemical Engineering 2024年第5期69卷 143-151页

作者： Wencai Ye Yulu Li Yonggang Dong Lin Yang Yun Yi Jianxin Cao School of Chemistry and chemical Engineering Guizhou UniversityGuiyang 550025China Engineering Research Center of Efficient Utilization for Industrial Waste Guizhou UniversityGuiyang 550025China key laboratory of guizhou Province for green chemical Industry and clean energy technology Guizhou UniversityGuiyang 550025China

The freezing acidolysis solution of the nitric acid-phosphate fertilizer process has a high calcium content,which makes it difficult to produce fine phosphate and high water-soluble phosphate fertilizer ***,based on the potential crystallization principle of calcium sulfate in NH_(4)NO_(3)-H_(3)PO_(4)-H_(2)O,the deep decalcification(*** removal)technology to achieveα-high-strength gypsum originated from freezing acidolysis-solutions has been firstly proposed and ***,calcium can be removed from the factory-provided freezing acidolysis-solution by neutralizing it with ammonia,followed by the addition of ammonium sulfate *** a result,the formation of calcium sulfate in the reaction system undergoes the nucleation and growth of CaSO_(4)·2H_(2)O(DH),as well as its dissolution and crystallization into short columnarα-CaSO_(4)·0.5H_(2)O(α-HH).Remarkably,with the molar ratio of SO_(4)^(2-)/Ca^(2+)at 1.8,the degree of neutralization(NH_(3)/HNO_(3) molar ratio)at 1.7,the reaction temperature of 94℃,and the reaction time of 300 min,the decalcification rate can reach 86.89%,of which the high-strengthα-CaSO_(4)·0.5H_(2)O(α-HH)will be ***,the deep decalcification product meets the standards for the production of fine phosphates and highly water-soluble phosphate ***,the 2 h flexural strength ofα-HH is 5.3 MPa and the dry compressive strength is 36.8 MPa,which is up to the standard of commercialα-HH.

关键词： Nitrophosphate Ammonia neutralization Deep decalcification High-strengthα-hemihydrate gypsum Controlled crystallization at atmospheric pressure

Effect of anions from calcium sources on the synthesis of nano-sized xonotlite fibers

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Optoelectronics Letters 2017年第2期13卷 81-83页

作者：刘飞陈莎林倩王晓丹曹建新 School of Chemistry and chemical Engineering Guizhou University Guiyang 550025 China key laboratory of green chemical and clean energy technology Guiyang 550025 China key laboratory of Efficient Utilization of Mineral and green chemical technology Guiyang 550025 China

The xonotlite fibers were synthesized via the hydrothermal synthesis method with CaO and SiO_2 as the raw materials and the molar ratio of Si/Ca of 1.0. Effect of anions from various calcium sources on the microstructure of the xonotlite fibers is studied in this paper. These obtained products were characterized by X-ray diffraction(XRD), transmission electron microscope(TEM) and scanning electron microscope(SEM) techniques to investigate their crystalline phase, crystal structure and morphology. The results indicate that anion from various calcium sources has little influence on the crystalline phases of xonotlite fibers but poses a great impact on their morphologies. Xonotlite fibers with single crystal characteristics and large aspect ratio of 50—100 were successfully fabricated from CaCl_2 as calcium material at 225 °C for 15 h. The existence of Cl-anion in the CaO-SiO_2-H_2O system significantly contributes to the formation of xonotlite crystal.

关键词： crystalline sized hydrothermal molar anion fibrous silica mixing crystallized colloidal

Research progress of catalysts for direct coal liquefaction

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Journal of energy Chemistry 2025年第1期 481-497页

作者： Wei Song Penggao Liu Xinyue Chen Ting Wang Chunrong He Rui Hao Kaiyu Liu State key laboratory of Chemistry and Utilization of Carbon Based energy Resources College of Chemistry Xinjiang University College of Chemistry and chemical Engineering Henan Polytechnic University Hunan provincial key laboratory of chemical Power Sources College of Chemistry and Chemical Engineering Central South University

Coal direct liquefaction technology is a crucial contemporary coal chemical technology for efficient and clean use of coal resources. The development of direct coal liquefaction technology and the promotion of alternative energy sources are important measures to guarantee energy security and economic security. However, several challenges need to be addressed, including low conversion rate, inadequate oil yield, significant coking, demanding reaction conditions, and high energy consumption. Extensive research has been conducted on these issues, but further exploration is required in certain aspects such as pyrolysis of macromolecules during the liquefaction process, hydrogen activation, catalysts' performance and stability, solvent hydrogenation, as well as interactions between free radicals to understand their mechanisms better. This paper presents a comprehensive analysis of the design strategy for efficient catalysts in coal liquefaction, encompassing the mechanism of coal liquefaction, catalyst construction,and enhancement of catalytic conversion efficiency. It serves as a comprehensive guide for further research endeavors. Firstly, it systematically summarizes the conversion mechanism of direct coal liquefaction, provides detailed descriptions of various catalyst design strategies, and especially outlines the catalytic mechanism. Furthermore, it addresses the challenges and prospects associated with constructing efficient catalysts for direct coal liquefaction based on an understanding of their action mechanisms.

关键词：

A Li_(3)P nanoparticle dispersion strengthened ultrathin Li metal electrode for high energy density rechargeable batteries

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Nano Research 2024年第5期17卷 4031-4038页

作者： Lin Fu Xiancheng Wang Bao Zhang Zihe Chen Yuanjian Li Yongming Sun provincial guizhou key laboratory of green chemical and clean energy technology School of Chemistry and Chemical EngineeringGuizhou UniversityGuiyang 550025China Wuhan National laboratory for Optoelectronics Huazhong University of Science and TechnologyWuhan 430074China School of Physical and Mathematical Sciences Nanyang Technological UniversitySingapore 637371Singapore Institute of Materials Research and Engineering Agency for Science Technology and Research(A*STAR)Singapore 138634Singapore

Achievement of lithium(Li)metal anode with thin thickness(e.g.,≤30µm)is highly desirable for rechargeable high energy density ***,the fabrication and application of such thin Li metal foil electrode remain challenging due to the poor mechanical processibility and inferior electrochemical performance of metallic ***,mechanico-chemical synthesis of robust ultrathin Li/Li_(3)P(LLP)composite foils(~15µm)is demonstrated by employing repeated mechanical rolling/stacking operations using red P and metallic Li as raw *** in-situ formed Li+-conductive Li_(3)P nanoparticles in metallic Li matrix and their tight bonding strengthen the mechanical durability and enable the successful fabrication of free-standing ultrathin Li metal composite ***,it also reduces the electrochemical Li nucleation barrier and homogenizes Li plating/stripping *** matching to high-voltage LiCoO_(2),the full cell with a low negative/positive(N/P)capacity ratio of~1.5 offers a high energy density of~522 W·h·kg^(-1) at 0.5 C based on the mass of cathode and *** into account its facile manufacturing,potentially low cost,and good electrochemical performance,we believe that such an ultrathin composite Li metal foil design with nanoparticle-dispersion-strengthened mechanism may boost the development of high energy density Li metal batteries.

关键词： lithium metal anode high energy density battery mechanico-chemical synthesis ultrathin Li/Li_(3)P composite foil low negative/positive capacity ratio