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Metal-Free PAZE-NH4X3⋅H2O Perovskite for Flexible Transparent X-ray Detection and Imaging

Angewandte Chemie 2022年第36期134卷

作者： Dr. Zhizai Li Dr. Guoqiang Peng Dr. Huanyu Chen Dr. Chang Shi Prof. ZhenHua Li Prof. Zhiwen Jin School of Physical Science and Technology & College of Chemistry and Chemical Engineering & Key Laboratory for Magnetism and Magnetic Materials of the Ministry of Education Lanzhou University Lanzhou 730000 China Contribution: Conceptualization (lead) Investigation (lead) Writing - original draft (lead) Contribution: Methodology (equal) Contribution: Methodology (supporting) School of Physical Science and Technology & Lanzhou Center for Theoretical Physics & Key Laboratory of Theoretical Physics of Gansu Province Lanzhou University Lanzhou 730000 China Contribution: Data curation (lead) Methodology (lead) Visualization (equal)

Metal-free perovskites are of interest for their chemical diversity and eco-friendly properties, and recently have been used for X-ray detection with superior carrier behavior. However, the size and shape complexity of the organic components results in difficulties in evaluating their stability in high-energy radiation. Herein, we introduce multiple hydrogen-bond metal-free PAZE-NH 4 X 3 ⋅H 2 O perovskite, where H 2 O leads to more hydrogen bonds appearing between organic molecules and the perovskite host. As suggested by the theoretical calculations, multiple hydrogen bonds promote stiffness of the lattice, and increase the diffusion barrier to inhibit ionic migration. Then, low trap density, high μτ products and structural flexibility of PAZE-NH 4 Br 3 ⋅H 2 O give a flexible X-ray detector with the highest sensitivity of 3708 μC Gy air −1 cm −2 , ultra-low detection limit of 0.19 μGy air −1 s −1 and superior spatial resolution of 5.0 lp mm −1 .

关键词： Metal-Free Hydrogen Bonds Imaging Perovskites X-Ray Detection

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Tunable schiff-based networks with different bonding sites for enhanced photocatalytic activity under visible-light irradiation: The effects of steric hindrance

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Environmental research 2024年 246卷 118200页

作者： Han Wang Piao Xu Eydhah Almatrafi Ziwei Wang Chengyun Zhou Ting Xiong Hong Qin Yangzhuo He Hailan Yang Zhuotong Zeng Guangming Zeng School of Metallurgy and Environment Central South University Changsha 410083 China Department of Dermatology Second Xiangya Hospital Central South University Changsha 410011 China College of Environmental Science and Engineering and Key Laboratory of Environmental Biology and Pollution Control (Ministry of Education) Hunan University Changsha 410082 China Center of Research Excellence in Renewable Energy and Power Systems Center of Excellence in Desalination Technology Department of Mechanical Engineering King Abdulaziz University Jeddah 21589 Saudi Arabia. College of Environmental Science and Engineering and Key Laboratory of Environmental Biology and Pollution Control (Ministry of Education) Hunan University Changsha 410082 China. Institute of Big Data and Internet Innovation Hunan University of Technology and Business Changsha 410205 China. Center of Research Excellence in Renewable Energy and Power Systems Center of Excellence in Desalination Technology Department of Mechanical Engineering King Abdulaziz University Jeddah 21589 Saudi Arabia. Electronic address: zgming@***.

Organic polymers hold great potential in photocatalysis considering their low cost, structural tailorability, and well-controlled degree of conjugation for efficient electron transfer. Among the polymers, Schiff base networks (SNWs) with high nitrogen content have been noticed. Herein, a series of SNWs is synthesized based on the melamine units and dialdehydes with different bonding sites. The chemical and structural variation caused by steric hindrance as well as the related photoelectric properties of the SNW samples are investigated, along with the application exploration on photocatalytic degradation and energy production. The results demonstrate that only SNW-o based on o-phthalaldehyde responds to visible light, which extends to over 550 nm. SNW-o shows the highest tetracycline degradation rate of 0.02516 min, under 60-min visible light irradiation. Moreover, the HO production of SNW-o is 2.14 times higher than that of g-CN. The enhanced photocatalytic activity could be ascribed to the enlarged visible light adsorption and intramolecular electron transfer. This study indicates the possibility to regulate the optical and electrical properties of organic photocatalysts on a molecular level, providing an effective strategy for rational supramolecular engineering to the applications of organic materials in photocatalysis.

关键词： H(2)O(2) production Photocatalytic degradation Schiff-based networks Steric hindrance Structure tunability

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Crystallization Regulation by Self-Assembling Liquid Crystal Template Enables Efficient and Stable Perovskite Solar Cells

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Angewandte Chemie 2023年第52期135卷

作者： Meizi Wu Hongyan Wang Yong Li Dr. Ran Chen Hui Zhou Shaomin Yang Dongfang Xu Kun Li Prof. Dr. Zhongwei An Shengzhong (Frank) Liu Prof. Dr. Zhike Liu Key Laboratory of Applied Surface and Colloid Chemistry Ministry of Education Shaanxi Key Laboratory for Advanced Energy Devices Shaanxi Engineering Lab for Advanced Energy Technology International Joint Research Center of Shaanxi Province for Photoelectric Materials Science School of Materials Science & Engineering Shaanxi Normal University Xi'an 710119 P. R. China Contribution: Data curation (lead) Formal analysis (lead) Investigation (lead) Writing - original draft (lead) Contribution: Data curation (equal) Formal analysis (equal) Contribution: Data curation (equal) Investigation (equal) School of Materials Science and Engineering Xi' an University of Science and Technology Xi'an 710054 P. R. China Contribution: Conceptualization (lead) Methodology (equal) Contribution: Formal analysis (equal) Investigation (equal) Contribution: Methodology (equal) Contribution: Data curation (equal) Contribution: Investigation (equal) Contribution: Conceptualization (equal) Methodology (equal) Contribution: Conceptualization (equal) Methodology (equal) Writing - review & editing (lead)

It is found that the disordered growth of bottom perovskite film deteriorates the buried interface of perovskite solar cells (PSCs), so developing a new material to modify the buried interface for regulating the crystal growth and defect passivation is an effective approach for improving the photovoltaic performance of PSCs. Here, we developed a new ionic liquid crystal (ILC, 1-Dodecyl-3-methylimidazolium tetrafluoroborate) as both crystal regulator and defect passivator to modify the buried interface of PSCs. The high lattice matching between this ILC and perovskite promotes preferential growth of perovskite film along [001] direction, while the oriented ILC with mesomorphic phase has a strong chemical interaction with perovskite to passivate the interface defect, as a result, the modified buried interface exhibits suppressed defects, improved band alignment, reduced nonradiative recombination losses, and enhanced charge extraction. The ILC-modified PSC delivers a power conversion efficiency of 24.92 % and maintains 94 % of the original value after storage in ambient for 3000 h.

关键词： Crystallization Regulation Ionic Liquid Crystals Perovskite Solar Cells Self-Assembling

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Wide Band-Gap Polymer Donors Functionalized with Unconventional Carbamate Side Chains for Polymer Solar Cells

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Angewandte Chemie 2022年第50期134卷

作者： Jie Tang Chentong Liao Yuwei Duan Xiaopeng Xu Min Deng Liyang Yu Ruipeng Li Qiang Peng School of Chemical Engineering College of Chemistry and State Key Laboratory of Polymer Materials Engineering Sichuan University Chengdu 610065 P. R. China Contribution: Conceptualization (equal) Data curation (lead) Formal analysis (lead) Methodology (lead) Contribution: Data curation (equal) Formal analysis (equal) Methodology (equal) Key Laboratory of Applied Surface and Colloid Chemistry of Ministry of Education Shaanxi Key Laboratory for Advanced Energy Devices Shaanxi Engineering Lab for Advanced Energy Technology School of Materials Science & Engineering Shaanxi Normal University Xi'an 710119 P. R. China Contribution: Data curation (supporting) Formal analysis (supporting) Contribution: Conceptualization (supporting) Data curation (supporting) Formal analysis (supporting) Contribution: Data curation (supporting) Formal analysis (supporting) Methodology (supporting) Contribution: Conceptualization (supporting) Formal analysis (supporting) Investigation (supporting) Supervision (supporting) Writing - original draft (lead) Writing - review & editing (supporting) National Synchrotron Light Source II Brookhaven National Lab Suffolk Upton NY 11973 USA Contribution: Conceptualization (lead) Project administration (lead) Supervision (lead) Validation (lead) Writing - review & editing (lead)

Side-chain engineering with heteroatoms is not only effective in tuning frontier molecular orbitals, but also possible for forming secondary bonds which can be utilized to planarize the molecular backbone, hence, improving the photon absorption as well as charge-transport abilities of polymer solar-cell (PSC) materials. Herein, two types of unconventional side chains, namely carboxylate and carbamate, containing various heteroatoms are introduced to the thiophene bridges in high performance benzodithiophene (BDT) based donor polymers to from the novel polymers PTzTz-C and PTzTz-N, respectively. In these polymers, non-covalent O⋅⋅⋅S and N⋅⋅⋅H interactions induce a high tendency to aggregation. In a ternary-blend PSC with PTzTz-N added to the high-performance D18 : BTP-eC9 blend, complimentary absorption and improved thin-film morphology were observed with a top power conversion efficiency of 18.76 %, which is an improvement of almost 5 % over the D18 : BTP-eC9 binary blends.

关键词： Carbamate Conformation Locks Donor Polymer Solar Cells

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The 2nd International Conference on Agricultural and Biological Sciences (ABS 2016)

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BMC Plant Biology 2016年第2期16卷 83-88页

作者： Lei Pei Zhenhua Wang Jinzhu Zhang Wenhao Li Adeline S. Y. Ting Yiing Y. Chow Sadequr Rahman Rongchang Wei Zhang Hu Sidong Li Chuyan Li Zijuan Li Guoxia Wang Yuzhen Yang Gang Chen Qing Luo Ruixia Liu Lipei Chen Zhiyang Lie Tongtong Zhou Weilong Huang Li Xue Jie Li Zhuomin Wang Ismail Bezirganoglu Pınar Uysal Shuihua Wang Zhihai Lu Jiquan Yang Yudong Zhang John Liu Ling Wei Shufang Chen Preetha Phillips Zhengchao Dong Hong Li Xutong Wang Fengliang Zhao Guisheng Yang Haijie Huang Weijian Huang Jinhui Wang Zhongrun Zhang Li Zhao Xiaojuan Li Ning Xu Guofu Zhou Ming Wan Fanyun Meng Jianxiu Li Qi Lin Yichang Chen Koayung Yu Chunpin Chang Zijuan Zhou Peixi Su Rui Shi Tingting Xie Xuelan Liu Yan Zhang Xiangfa Wei Chong Wu Yanlei Yin Lijuan Feng Xuemei Yang Fei Wang Hua Wang Huifa Zhuang Zihui Zhu Hui Wang College of Water & Architectural Engineering Shihezi University Shihezi City 832000 Xinjiang China Key Laboratory of Modern Water-Saving Irrigation Corp Shihezi University Shihezi City 832000 Xinjiang China School of Science Monash University Malaysia Jalan Lagoon Selatan 46150 Bandar Sunway Selangor Malaysia Guangxi Botanical Garden of Medicinal Plants Nanning Guangxi Province 530023 China Department of Chemistry College of Science Guangdong Ocean University Zhanjiang 524088 China School of Life Science Zhengzhou Normal University Zhengzhou 450044 China College of Forestry and Landscape Architecture South China Agricultural University Guangzhou 510642 China Deparment of Molecular Biology and Genetic Erzurum Technical University Erzurum 442 Turkey Ministry of Food Agriculture and Husbandry Eastern Anatolia Agriculture Research Institute Erzurum 442 Turkey Nanjing Normal University Nanjing Jiangsu 210023 China Key laboratory of symbolic computation and knowledge engineering of ministry of education Jilin University Changchun Jilin 130012 China Michigan State University East Lansing MI 48823 USA Shanghai Jiaotong University Shanghai 200030 China University of Electronic Science and Technology of China Chengdu Sichuan 611731 China Shepherd University Shepherdstown WV 25443 USA West Virginia University Morgantown WV 26505 USA New York State Psychiatric Institute New York NY 10032 USA Environment and Plant Protection Institute Chinese Academy of Tropical Agricultural Science Haikou Hainan 571101 China Tropical Crops Genetic Resources Institute CATAS Danzhou 571737 China College of Applied Science and Technology Hainan University Danzhou 571737 China Beijing Area Major Laboratory of Protection and Utilization of Traditional Chinese Medicine Beijing Normal University Beijing 100875 China State Key Laboratory Breeding Base of Dao-di Herbs National Resource Center for Chinese Materia Medica China Academy of Chinese Medical Science

01 The influence of soil salt content on the photosynthetic characteristics of spring wheat with trickle irrigationLei Pei, Zhenhua Wang, Jinzhu Zhang, Wenhao Li02 Comparing growth of fast-growing and slow-growing end... 详细信息

01 The influence of soil salt content on the photosynthetic characteristics of spring wheat with trickle irrigation

Lei Pei, Zhenhua Wang, Jinzhu Zhang, Wenhao Li

02 Comparing growth of fast-growing and slow-growing endophytes in plants via ergosterol quantification

Adeline SY Ting, Yiing Y Chow, Sadequr Rahman

03 Transcriptome and digital gene expression analysis identifies putative triterpene saponin-biosynthetic genes of Panax notoginseng

Rongchang Wei

04 Chitosan-assisted isolation and antioxidant evaluation of flavonoids from Sophora japonica L.

Zhang Hu, Sidong Li, Chuyan Li, Zijuan Li

05 Two kinds of new characteristics of the ektexine ornamentation of ginkgo pollen

Guoxia Wang, Yuzhen Yang, Gang Chen, Qing Luo

06 Analysis of nutrient and medicinal ingredients of Ginkgo pollen in different regions

Guoxia Wang, Ruixia Liu, Yuzhen Yang, Lipei Chen

07 Photosynthetic performance of greening seedlings of seven species to drought stress

Zhiyang Lie, Tongtong Zhou, Weilong Huang, Li Xue

08 Changes of fluorescence parameters of greening seedlings of seven species under drought stress

Jie Li, Zhuomin Wang, Li Xue

09 Mammalian sex hormone affects regeneration capacity and enzymes activity of Triticale L in vitro culture

Ismail Bezirganoglu, Pınar Uysal

10 Fractional Fourier entropy increases the recognition rate of fruit type detection

Shuihua Wang, Zhihai Lu, Jiquan Yang, Yudong Zhang, John Liu, Ling Wei, Shufang Chen, Preetha Phillips, Zhengchao Dong

11 Banana-peanut intercropping reduces Fusarium wilt disease in banana from enhancing soil bacterial microorganisms and leaf nutrition

Hong Li, Xutong Wang, Fengliang Zhao, Guisheng Yang

12 Manganese stress impairs stem ureide nitrogen fixation in yardlong-bean plants in the acidic environment

Hong Li

13 A new

关键词： Spring Wheat Vanilla Panax Notoginseng Soil Salt Content Digital Gene Expression Analysis

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A Targeting Singlet Oxygen Battery for Multidrug-Resistant Bacterial Deep-Tissue Infections

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Angewandte Chemie 2023年第36期135卷

作者： Yiwen Zhu Minzheng Gao Mengrui Su Yanzhe Shen Kai Zhang Bingran Yu Fu-Jian Xu State Key Laboratory of Chemical Resource Engineering Key Lab of Biomedical Materials of Natural Macromolecules (Beijing University of Chemical Technology Ministry of Education) Laboratory of Biomedical Materials Beijing University of Chemical Technology Beijing 100029 China Contribution: Methodology (equal) Software (equal) Writing - original draft (lead) Contribution: Methodology (equal) Software (equal) Writing - original draft (equal) Contribution: Methodology (equal) Contribution: Methodology (supporting) Contribution: Data curation (lead) Contribution: Conceptualization (lead) Funding acquisition (equal) Writing - review & editing (lead)

Traditional photodynamic therapy (PDT) is dependent on externally applied light and oxygen, and the depth of penetration of these factors can be insufficient for the treatment of deep infections. The short half-life and short diffusion distance of reactive oxygen species (ROS) also limit the antibacterial efficiency of PDT. Herein, we designed a targeting singlet oxygen delivery system, CARG-Py, for irradiation-free and oxygen-free PDT. This system was converted to the “singlet oxygen battery” CARG- 1 O 2 and released singlet oxygen without external irradiation or oxygen. CARG- 1 O 2 is composed of pyridones coupled to a targeting peptide that improves the utilization of singlet oxygen in deep multidrug-resistant bacterial infections. CARG- 1 O 2 was shown to damage DNA, protein, and membranes by increasing the level of reactive oxygen inside bacteria; the attacking of multiple biomolecular sites caused the death of methicillin-resistant Staphylococcus aureus (MRSA). An in vivo study in a MRSA-infected mouse model of pneumonia demonstrated the potential of CARG- 1 O 2 for the efficient treatment of deep infections. This work provides a new strategy to improve traditional PDT for irradiation- and oxygen-free treatment of deep infections while improving convenience of PDT.

关键词： Antibacterial Mechanism Deep-Tissue Infections Multidrug-Resistant Singlet Oxygen Battery Targeting Therapy

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Corrigendum to “Oscillation-free source term inversion of atmospheric radionuclide releases with joint model bias corrections and non-smooth competing priors” [J. Hazard. Mater. 440 (2022) 129806]

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Journal of Hazardous Materials 2023年 445卷

作者： Sheng Fang Xinwen Dong Shuhan Zhuang Zhijie Tian Tianfeng Chai Yuhan Xu Yungang Zhao Li Sheng Xuan Ye Wei Xiong Institute of Nuclear and New Energy Technology Collaborative Innovation Centre of Advanced Nuclear Energy Technology Key Laboratory of Advanced Reactor Engineering and Safety of Ministry of Education Tsinghua University Beijing 100084 China China Institute for Radiation Protection Taiyuan 030006 China NOAA Air Resources Laboratory (ARL) NOAA Center for Weather and Climate Prediction 5830 University Research Court College Park MD 20740 USA Cooperative Institute for Climate and Satellites University of Maryland College Park MD 20740 USA Key Laboratory of Beam Technology of Ministry of Education College of Nuclear Science and Technology Beijing Normal University Beijing 100875 China CTBT Beijing National Data Centre and Beijing Radionuclide Laboratory Beijing 100085 China CMA Earth System Modeling and Prediction Center (CEMC) Beijing 100081 China

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Influencing Factors on Li-ion Conductivity and Interfacial Stability of Solid Polymer Electrolytes, Exampled by Polycarbonates, Polyoxalates and Polymalonates

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Angewandte Chemie 2023年第13期135卷

作者： Dr. Xiaoxin Xie Prof. Zhaoxu Wang Dr. Shuang He Kejun Chen Qiu Huang Peng Zhang Prof. Shu-Meng Hao Dr. Jiantao Wang Prof. Weidong Zhou Beijing Advanced Innovation Center for Soft Matter Science and Engineering State Key Laboratory of Organic-Inorganic Composites Beijing University of Chemical Technology Beijing 100029 China Contribution: Data curation (lead) Investigation (lead) Writing - original draft (lead) Key Laboratory of Theoretical Organic Chemistry and Functional Molecule of Ministry of Education Hunan University of Science and Technology Hunan 411201 China Contribution: Data curation (equal) Investigation (supporting) Software (equal) Contribution: Investigation (supporting) Software (supporting) Contribution: Investigation (supporting) Contribution: Supervision (supporting) China Automotive Battery Research Institute Co. Ltd. Beijing 101407 China

The application of solid polymer electrolytes (SPEs) in all-solid-state(ASS) batteries is hindered by lower Li + -conductivity and narrower electrochemical window. Here, three families of ester-based F-modified SPEs of poly-carbonate (PCE), poly-oxalate (POE) and poly-malonate (PME) were investigated. The Li + -conductivity of these SPEs prepared from pentanediol are all higher than the counterparts made of butanediol, owing to the enhanced asymmetry and flexibility. Because of stronger chelating coordination with Li + , the Li + -conductivity of PME and POE is around 10 and 5 times of PCE. The trifluoroacetyl-units are observed more effective than −O−CH 2 −CF 2 −CF 2 −CH 2 −O− during the in situ passivation of Li-metal. Using trifluoroacetyl terminated POE and PCE as SPE, the interfaces with Li-metal and high-voltage-cathode are stabilized simultaneously, endowing stable cycling of ASS Li/LiNi 0.6 Co 0.2 Mn 0.2 O 2 (NCM622) cells. Owing to an enol isomerization of malonate, the cycling stability of Li/PME/NCM622 is deteriorated, which is recovered with the introduce of dimethyl-group in malonate and the suppression of enol isomerization. The coordinating capability with Li + , molecular asymmetry and existing modes of elemental F, are all critical for the molecular design of SPEs.

关键词： All-Solid-State Battery High Voltage Cathode Interfacial Stability Lithium Metal Anode Solid Polymer Electrolyte

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Fluorine-Containing Passivation Layer via Surface Chelation for Inorganic Perovskite Solar Cells

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Angewandte Chemie 2022年第6期135卷

作者： Hao Zhang Prof. Wanchun Xiang Xuejiao Zuo Xiaojing Gu Shiang Zhang Yachao Du Zhiteng Wang Yali Liu Haifeng Wu Peijun Wang Qingyue Cui Hang Su Prof. Qingwen Tian Prof. Shengzhong (Frank) Liu Key Laboratory of Applied Surface and Colloid Chemistry Ministry of Education Shaanxi Key Laboratory for Advanced Energy Devices Shaanxi Engineering Lab for Advanced Energy Technology School of Materials Science and Engineering Shaanxi Normal University No. 620 West Chang'an Avenue Xi'an 710119 P. R. China Contribution: Data curation (lead) Formal analysis (lead) Investigation (lead) Writing - original draft (supporting) Contribution: Conceptualization (lead) Data curation (lead) Writing - original draft (lead) Contribution: Formal analysis (supporting) Investigation (supporting) Contribution: Data curation (supporting) Formal analysis (equal) Investigation (equal) Contribution: Data curation (supporting) Investigation (supporting) Contribution: Data curation (supporting) Formal analysis (supporting) State Key Laboratory of Organic-Inorganic Composites Key Lab of Biomedical Materials of Natural Macromolecules Ministry of Education Beijing Laboratory of Biomedical Materials Beijing University of Chemical Technology No. 15 East Road North Third Ring Chaoyang District Beijing 100029 P. R. China Contribution: Conceptualization (lead) Data curation (lead) Funding acquisition (lead) Project administration (lead) Supervision (lead) Validation (lead) Visualization (lead) Writing - review & editing (lead) Dalian National Laboratory for Clean Energy iChEM Dalian Institute of Chemical Physics Chinese Academy of Sciences No. 457 Zhongshan Road Dalian Liaoning 116023 P. R. China Contribution: Project administration (lead) Supervision (lead) Validation (lead) Writing - review & editing (equal)

Minimizing surface defect is vital to further improve power conversion efficiency (PCE) and stability of inorganic perovskite solar cells (PSCs). Herein, we designed a passivator trifluoroacetamidine (TFA) to suppress CsPbI 3− x Br x film defects. The amidine group of TFA can strongly chelate onto the perovskite surface to suppress the iodide vacancy, strengthened by additional hydrogen bonds. Moreover, three fluorine atoms allow strong intermolecular connection via intermolecular hydrogen bonds, thus constructing a robust shield against moisture. The TFA-treated PSCs exhibit remarkably suppressed recombination, yielding the record PCEs of 21.35 % and 17.21 % for 0.09 cm 2 and 1.0 cm 2 device areas, both of which are the highest for all-inorganic PSCs so far. The device also achieves a PCE of 39.78 % under indoor illumination, the highest for all-inorganic indoor photovoltaic devices. Furthermore, TFA greatly improves device ambient stability by preserving 93 % of the initial PCE after 960 h.

关键词： Chelation Defect Passivation Inorganic Perovskite Solar Cells

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Amorphous Mo-doped NiS0.5Se0.5Nanosheets@Crystalline NiS0.5Se0.5Nanorods for High Current-density Electrocatalytic Water Splitting in Neutral Media

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Angewandte Chemie 2022年第6期135卷

作者： Dr. Yang Wang Dr. Xiaopeng Li Dr. Zhong Huang Dr. Haozhi Wang Dr. Zelin Chen Dr. Jinfeng Zhang Prof. Xuerong Zheng Prof. Yida Deng Prof. Wenbin Hu State Key Laboratory of Marine Resource Utilization in South China Sea School of Materials Science and Engineering Hainan University Haikou 570228 P. R. China Contribution: Data curation (lead) Investigation (lead) Methodology (lead) Validation (lead) Writing - original draft (lead) School of Materials Science and Engineering Tianjin Key Laboratory of Building Green Functional Materials Tianjin Chengjian University Tianjin 300384 China Contribution: Formal analysis (equal) State Key Laboratory of Marine Resource Utilization in South China Sea College of Information and Communication Engineering Hainan University Haikou 570228 P. R. China Contribution: Methodology (equal) Software (equal) Validation (equal) Contribution: Methodology (equal) Software (equal) School of Materials Science and Engineering Tianjin Key Laboratory of Composite and Functional Materials Key Laboratory of Advanced Ceramics and Machining Technology of Ministry of Education Tianjin University Tianjin 300072 P. R. China Contribution: Methodology (equal) Contribution: Conceptualization (equal) Investigation (equal) Supervision (equal) Contribution: Funding acquisition (lead) Supervision (equal) Contribution: Funding acquisition (supporting)

It is vitally important to develop highly active, robust and low-cost transition metal-based electrocatalysts for overall water splitting in neutral solution especially at large current density. In this work, amorphous Mo-doped NiS 0.5 Se 0.5 nanosheets@crystalline NiS 0.5 Se 0.5 nanorods (Am−Mo−NiS 0.5 Se 0.5 ) was synthesized using a facil one-step strategy. In phosphate buffer saline solution, the Am−Mo−NiS 0.5 Se 0.5 shows tiny overpotentials of 48 and 209 mV for hydrogen evolution reaction (HER), 238 and 514 mV for oxygen evolution reaction (OER) at 10 and 1000 mA cm −2 , respectively. Moreover, Am−Mo−NiS 0.5 Se 0.5 delivers excellent stability for at least 300 h without obvious degradation. Theoretical calculations revealed that the Ni sites in the defect-rich amorphous structure of Am−Mo−NiS 0.5 Se 0.5 owns higher electron state density and strengthened the binding energy of H 2 O, which will optimize H adsorption/desorption energy barriers and reduce the adsorption energy of OER determining step.

关键词： Amorphous Crystalline High-Current-Density Neutral Environment Water Splitting

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