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Accelerating the Screening of Modified MA_(2)Z_(4) Catalysts for Hydrogen Evolution Reaction by Deep Learning-Based Local Geometric Analysis

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Energy & Environmental Materials 2024年第6期7卷 290-302页

作者： Jingnan Zheng Shibin Wang Shengwei Deng zihao yao Junhua Hu Jianguo Wang Institute of Industrial Catalysis State Key Laboratory Breeding Base of Green-Chemical Synthesis TechnologyCollege of Chemical EngineeringZhejiang University of TechnologyHangzhou 310032China School of Materials Science and Engineering Zhengzhou UniversityZhengzhou 450001China School of Materials Science and Engineering State Center for International Cooperation on Designer Low-Carbon&Environmental Materials(CDLCEM)Zhengzhou UniversityZhengzhou 450001China

Machine learning(ML)integrated with density functional theory(DFT)calculations have recently been used to accelerate the design and discovery of single-atom catalysts(SACs)by establishing deep structure–activity *** traditional ML models are always difficult to identify the structural differences among the single-atom systems with different modification methods,leading to the limitation of the potential application *** to the structural properties of several typical two-dimensional MA_(2)Z_(4)-based single-atom systems(bare MA_(2)Z_(4) and metal single-atom doped/supported MA_(2)Z_(4)),an improved crystal graph convolutional neural network(CGCNN)classification model was employed,instead of the traditional machine learning regression model,to address the challenge of incompatibility in the studied *** CGCNN model was optimized using crystal graph representation in which the geometric configuration was divided into active layer,surface layer,and bulk layer(ASB-GCNN).Through ML and DFT calculations,five potential single-atom hydrogen evolution reaction(HER)catalysts were screened from chemical space of 600 MA_(2)Z_(4)-based materials,especially V_(1)/HfSn_(2)N_(4)(S)with high stability and activity(Δ_(GH*)is 0.06 eV).Further projected density of states(pDOS)analysis in combination with the wave function analysis of the SAC-H bond revealed that the SAC-dz^(2)orbital coincided with the H-s orbital around the energy level of−2.50 eV,and orbital analysis confirmed the formation ofσ*** study provides an efficient multistep screening design framework of metal single-atom catalyst for HER systems with similar two-dimensional supports but different geometric configurations.

关键词： graph convolutional neural network hydrogen evolution reaction modified MA_(2)Z_(4) substrate single atom catalyst

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Building highly active hybrid double-atom sites in C_(2)N for enhanced electrocatalytic hydrogen peroxide synthesis

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Green Energy & Environment 2021年第6期6卷 846-857页

作者： Yongyong Cao JinYan Zhao Xing Zhong Guilin Zhuang Shengwei Deng Zhongzhe Wei zihao yao Jianguo Wang College of Biological Chemical Science and Engineering Jiaxing UniversityJiaxing314001China Institute of Industrial Catalysis College of Chemical EngineeringState Key Laboratory Breeding Base of Green–Chemical Synthesis TechnologyZhejiang University of TechnologyHangzhou310032China

Two-electron(2 e^(-))oxygen reduction reaction(ORR)shows great promise for on-site electrochemical synthesis of hydrogen peroxide(H_(2)O_(2)).However,it is still a great challenge to design efficient electrocatalysts for H_(2)O_(2)*** address this issue,the logical design of the active site by controlling the geometric and electronic structures is urgently ***,using density functional theory(DFT)computations,two kinds of hybrid double-atom supported on C_(2)N nanosheet(RuCu@C_(2)N and PdCu@C_(2)N)are screened out and their H_(2)O_(2)performances are ***@C_(2)N exhibits higher activity for H_(2)O_(2)synthesis with a lower overpotential of 0.12 V than RuCu@C_(2)N(0.59 V),Ru_(3)Cu(110)facet(0.60 V),and PdCu(110)facet(0.54 V).In aqueous phase,the adsorbed O_(2)is further stabilized with bulk H_(2)0 and the thermodynamic rate-determining step of 2 e^(-) ORR *** activation barrier on PdCu@C_(2)N is 0.43 eV lower than the one on RuCu@C_(2)N with 0.68 ***@C_(2)N is near the top of 2 e^(-) ORR volcano plot,and exhibits high selectivity of H_(2)O_(2.)This work provides guidelines for designing highly effective hybrid double-atom electrocatalysts(HDACs)for H_(2)O_(2)synthesis.

关键词： Hydrogen peroxide(H_(2)O_(2)) Oxygen reduction reaction(ORR) Hybrid double-atoms catalysts(HDACs) Density functional theory(DFT) Aqueous phase

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A generalized formula for two-dimensional diffusion of CO in graphene nanoslits with different Pt loadings

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Green Energy & Environment 2020年第3期5卷 322-332页

作者： Chenglong Qiu Yinbin Wang Yuejin Li Xiang Sun Guilin Zhuang zihao yao Shengwei Deng Jianguo Wang Institute of Industrial Catalysis State Key Laboratory Breeding Base of Green-Chemical Synthesis TechnologyCollege of Chemical EngineeringZhejiang University of TechnologyHangzhou310032China

Catalytic performance of supported metal catalysts not only depends on the reactivity of metal,but also the adsorption and diffusion properties of gas molecules which are usually affected by many factors,such as temperature,pressure,properties of metal clusters and substrates,*** explore the impact of each of these macroscopic factors,we simulated the movement of CO molecules confined in graphene nanoslits with or without supported Pt *** results of molecular dynamics simulations show that the diffusion of gas molecules is accelerated with high temperature,low pressure or low surface-atom number of supported ***,the supported metal nanoparticles greatly affect the gas diffusion due to the adsorption of gas ***,to bridge a quantitative relationship between microscopic simulation and macroscopic properties,a generalized formula is derived from the simulation data to calculate the diffusion *** work helps to advise the diffusion modulation of gas molecules via structural design of catalysts and regulation of reaction conditions.

关键词： Gas diffusion Graphene nanoslits Supported Pt nanoparticles Molecular dynamics simulation

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The Structural and Chemical Reactivity of Lattice Oxygens on β-PbO_(2 ) EOP Electrocatalysts

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Chinese Journal of Structural Chemistry 2022年第12期41卷 51-59页

作者： Wenwen Li Ge Feng Jia Liu Xing Zhong zihao yao Shengwei Deng Shibin Wang Jianguo Wang Institute of Industrial Catalysis State Key Laboratory Breeding Base of Green-Chemical Synthesis TechnologyCollege of Chemical EngineeringZhejiang University of TechnologyHangzhou 310032P.R.China

The oxygen evolution reaction(OER)and electrochemical ozone production(EOP)attracted considerable attention due to their wide applications in electrocatalysis,but the detailed reaction mechanism of product formation as well as the voltage effect on O_(2)/O_(3)formation still remains *** this work,density functional theory calculations were used to systematically investigate the possible reaction mechanisms of OER and EOP on the PbO_(2)(110)surface,with the possible reaction network involving surface lattice oxygen atoms(LOM)*** results show that the LOM-2 reaction pathway involving two surface lattice oxygen atoms(Olatt)and one oxygen atom from H_(2)O was the most thermodynamically *** potential determining step(PDS)was obtained depending on the multiple reaction pathway,and the results show that the facile diffusion of Olattwould proceed the LOM pathway and promote the formation of surface oxygen vacancies(O_(vac1)/O_(vac2)).Furthermore,O_(vac1)/O_(vac2)formation on the surface would trigger further reactions of H_(2)O adsorption and splitting,which refilled the oxygen vacancy and ensured the considerable stability of the PbO_(2)(110)*** H_(2)O dissociation pathways were proposed on PbO_(2)(110)with oxygen vacancy sites:the acid-base interaction mechanism and the vacancy fulfilling mechanism.

关键词： oxygen vacancy effect electrochemical ozone production lattice oxygen mechanism density functional theory

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Synergistic effect of size-dependent PtZn nanoparticles and zinc single-atom sites for electrochemical ozone production in neutral media

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Journal of Energy Chemistry 2020年第12期29卷 312-322页

作者： Bowen Yuan zihao yao Chenlong Qiu Haiyang Zheng Yilong Yan Qiaoqiao Zhang Xiang Sun Yu Gu Xing Zhong Jianguo Wang Institute of Industrial Catalysis State Key Laboratory Breeding Base of Green-Chemical Synthesis TechnologyCollege of Chemical EngineeringZhejiang University of TechnologyHangzhou 310032ZhejiangChina

Electrochemical ozone production(EOP) via water electrolysis represents an attractive method for the generation of high-purity O3. Herein, the X-PtZn/Zn-N-C electrocatalysts show a strong structural sensitive behavior depends on the size of the PtZn nanoparticles and their EOP activity exhibits a volcano-type dependence for the O3 performance in neutral media. The 7.7-PtZn/Zn-N-C exhibits EOP current efficiency of 4.2%, and shows the prominent performance in the production of gaseous O3 with a value of 1647 ppb at 30 min, which is almost 4-fold compared to 2.2-Pt Zn/Zn-N-C. Based on the experiments and theoretical calculations, the performance of the EOP process was determined by the nanoparticle size-effect and the synergistic effect between the PtZn nanoparticles and atomically dispersed Zn-N-C. Furthermore, the fivemembered cyclic structure of O3 can be stabilized between the PtZn nanoparticle and the Zn-N-C support,indicating that O3 is produced at the interface.

关键词： Electrochemical ozone production PtZn Single-atom catalysts Size effect Synergistic effect

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Tuning the ratio of Bi/Bi_(2)O_(3)in Bi/PNC nanosheet for highefficiency electrosynthesis hydrogen peroxide

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Nano Research 2023年第7期16卷 9050-9058页

作者： Zhikang Bao Jinyan Zhao Shijie Zhang Xiaoge Peng Yizhen Shao Chenghang Jiang Zaixiang Xu Xing Zhong zihao yao Jianguo Wang Institute of Industrial Catalysis College of Chemical EngineeringState Key Laboratory Breeding Base of Green-Chemical Synthesis TechnologyZhejiang University of TechnologyHangzhou 310032China

Electrocatalytic two-electron oxygen reduction reaction(2e-ORR)is a promising method for producing green and sustainable H_(2)O_(2)but lacks high selectivity and yields *** it is critical to develop catalysts that meet industrial ***,we report the different ratios of Bi0/Bi^(3+)supported on a phosphorus,nitrogen,and carbon nanosheet(Bi/PNC),which can reduce O_(2) to H_(2)O_(2)with high selectivity(up to 97.75%at 0.4 VRHE)in 0.1 M KOH electrolyte and retain 97%selectivity even after 100 h *** a homemade flow-cell system was built for electrocatalytic production of H_(2)O_(2)under an O_(2) atmosphere using an improved gas diffusion *** Bi/PNC-4 can achieve a high H_(2)O_(2)yield of 2.76 mol·gcatalyst^(-1)·h^(-1)(alkaline),5.29 mol·gcatalyst^(-1)·h^(-1)(neutral),and 3.50 mol·gcatalyst^(-1)·h^(-1)(acid)in universal pH *** in-situ generated H_(2)O_(2)can function as a degradation agent for efficiently degrading pesticides and *** outstanding selectivity and activities are attributed to the synergistic effects of Bi0 and Bi^(3+)that promote proton-coupled reduction of O_(2) to OOH^(*)(ΔGOOH^(*)=4.27 eV),and the formation of H_(2)O_(2).The fast yield of H_(2)O_(2)on Bi/PNC catalysts in flow-cell provides a promising path of electrocatalytic 2e-ORR for practical H_(2)O_(2)production.

关键词： hydrogen peroxide nanosheet Bi_(2)O_(3) Bi degradation

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A first-principles study of reaction mechanism over carbon decorated oxygen-deficient TiO_(2) supported Pd catalyst in direct synthesis of H_(2)O_(2)

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Chinese Journal of Chemical Engineering 2021年第3期34卷 126-134页

作者： zihao yao Jinyan Zhao Chenxia Zhao Shengwei Deng Guilin Zhuang Xing Zhong Zhongzhe Wei Yang Li Shibin Wang Jianguo Wang Institute of Industrial Catalysis College of Chemical EngineeringZhejiang University of TechnologyHangzhou 310032China

The choice of support is one of the most significant components in the direct synthesis of H_(2)O_(2).Aiming to improvement of activity and selectivity of H_(2)O_(2) on Pd/TiO_(2) surface,we systematically investigated the important elementary steps on Pd/TiO_(2)-Vo@C,Pd/TiO_(2)-Vo,Pd/TiO_(2)-2 Vo,Pd/TiO_(2),and Pd/C using the first-principles *** Bader charge analysis and charge density difference of O_(2) adsorption elucidate the relationship between the electronic distribution and chemisorption *** effective barrier analysis further enables to quantitatively estimate the reactivity of H_(2)O_(2) and *** demonstrate unambiguously that the selectivity of H2O formation is boosted as the oxygen vacancy concentration ***,the introduction of C into a TiO_(2) with appropriate oxygen vacancies can slightly reduce the effective barrier for H_(2)O_(2) formation and increase the effective barrier for H2O formation leading to a higher activity and selectivity of H_(2)O_(2) *** finding suggests that carbon-doped oxygen vacancy TiO_(2) supported Pd is potential alternative catalyst compared with the Pd/TiO_(2).

关键词： Direct synthesis of H_(2)O_(2) DFT Supported Pd-catalysts TiO_(2)-support Carbon-doped Oxygen vacancies

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Trace water triggers high-efficiency photocatalytic hydrogen peroxide production

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Journal of Energy Chemistry 2022年第1期31卷 47-54,I0003页

作者： Zaixiang Xu Yang Li Yongyong Cao Renfeng Du Zhikang Bao Shijie Zhang Fangjun Shao Wenkai Ji jun Yang Guilin Zhuang Shengwei Deng Zhongzhe Wei zihao yao Xing Zhong Jianguo Wang Institute of Industrial Catalysis College of Chemical EngineeringState Key Laboratory Breeding Base of Green-Chemical Synthesis TechnologyZhejiang University of TechnologyHangzhou 310032ZhejiangChina Department of Chemistry Zhejiang UniversityHangzhou 310027ZhejiangChina

Photocatalytic production of hydrogen peroxide(H_(2)O_(2))has attracted much attentions as a promising method for sustainable solar ***,we demonstrate that trace water can drastically boost highefficiency photocatalytic production of H_(2)O_(2) with a record-high concentration of 113 mmol L^(-1) using alkali-assisted C_(3)N_(4) as photocatalyst in water/alcohol mixture *** electron paramagnetic resonance(EPR)measurement,the radical species generated during the photocatalytic process of H_(2)O_(2) are *** propose alcohol is used to provide and stabilize-OOH radicals through hydrogen bond,while trace water could trigger photocatalytic production of H_(2)O_(2) via providing and transferring indispensable free protons to completely consume OOH radicals,which breaks the reaction balance of-OOH radical generation from ***-OOH radicals could be supplied by alcohol continuously to serve as a reservoir for high-efficiency production of H_(2)O_(2).These results pave the way towards photocatalytic method on semiconductor catalysts as an outstanding approach for production of hydrogen peroxide.

关键词： Hydrogen peroxide Photocatalysis Carbon nitride Water Radicals

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“帮信罪”口袋化适用及其消减路径研究

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四川职业技术学院学报 2022年第5期32卷 22-27,35页

作者：姚自豪西南政法大学法学院重庆渝北401120

当下,“帮信罪”已成为网络犯罪治理中最常适用的罪名。梳理相关裁判文书可发现,司法裁判者过于依赖该罪名并逐渐“口袋化”适用,对“明知”“帮助”“情节严重”等要素的解释有诸多不当,可能会引发对行为类型的虚置,掩盖实际罪情。消... 详细信息

当下,“帮信罪”已成为网络犯罪治理中最常适用的罪名。梳理相关裁判文书可发现,司法裁判者过于依赖该罪名并逐渐“口袋化”适用,对“明知”“帮助”“情节严重”等要素的解释有诸多不当,可能会引发对行为类型的虚置,掩盖实际罪情。消减此现象应基于网络犯罪的特殊场域,合理解读“明知”的内涵及指向,并借助各类证据综合认定;定性“帮助”应关注基于技术特征所呈现的行为类型;并摆脱“刑法万能主义”的窠臼,树立综合治理的观念。

关键词：帮助信息网络犯罪活动罪口袋化适用消减路径

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网络服务提供者不作为犯罪类型的归结与厘清

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宜宾学院学报 2023年第4期23卷 60-67页

作者：姚自豪西南政法大学法学院重庆401120

“该为,能为,但不为”系不作为犯罪之成立路径,而作为义务的设置以作为能力为参照,作为可能的衡量以作为能力为标尺,因此,作为能力系成立不作为犯罪的重要评价依据。实践中网络服务提供者因技术功能不同而在作为能力水平上存在差异,而... 详细信息

“该为,能为,但不为”系不作为犯罪之成立路径,而作为义务的设置以作为能力为参照,作为可能的衡量以作为能力为标尺,因此,作为能力系成立不作为犯罪的重要评价依据。实践中网络服务提供者因技术功能不同而在作为能力水平上存在差异,而规范文本理想化地赋予所有网络服务提供者近乎一致的义务内容,忽视了不同主体间以技术功能为核心的种类差异,导致犯罪评价忽视个体差异、罪名选择和适用相对片面。正确的做法是设置以技术功能为核心的层次化区分标准,将网络服务提供者划分为内容类、中间类和其他复合类,考察不同主体在实施不作为犯罪时是否齐备保证人地位、作为能力和作为可能等要件内容,还需要在此基础上探究不同犯罪参与模式、义务模式以及主体模式下典型的不作为犯罪成立情形,以厘清网络服务提供者不作为犯罪成立的常见类型,避免不当归责。

关键词：网络服务提供者技术功能不作为犯罪类型

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