The electrochemical water splitting to produce hydrogen converts electric energy into clean hydrogen energy,which is a groundbreaking concept of energy optimization.To achieve high efficiency,numerous strategies have ...The electrochemical water splitting to produce hydrogen converts electric energy into clean hydrogen energy,which is a groundbreaking concept of energy optimization.To achieve high efficiency,numerous strategies have been developed to enhance the performance of electrocatalysts.Among these,interface engineering with molecules/ions/groups,serves as a versatile approach for optimizing the performance of electrocatalysts in water splitting.On the basis of numerous achievements in high-performance electrocatalysts engineered through molecules/ions/groups at interface,a comprehensive understanding of these advancements is crucial for guiding future progress.Herein,after providing a concise overview of the background,the interface engineering via molecules/ions/groups for electrocatalytic water splitting is demonstrated from three perspectives.Firstly,the engineering of electronic state of electrocatalysts by molecules/ions/groups at interface to reduce the Gibbs free energy of the corresponding reactions.Secondly,the modification of local microenvironment surrounding electrocatalysts via molecules/ions/groups at interface to enhance the transfer of reactants and products.Thirdly,the protection of electrocatalysts with molecule/ion/group fences improves their durability,including protecting active sites from leaching and defending them against harmful species.The fundamental principles of these three aspects are outlined for each,along with pertinent comments.Finally,several research directions and challenges are proposed.展开更多
This paper computes the group and character table of Trimethylborane and Cyclohaxane. Results show that the groups are isomorphic to the wreath products C3wrC2 and C2wrC6 with orders 81 and 384 and with 17 and 28 conj...This paper computes the group and character table of Trimethylborane and Cyclohaxane. Results show that the groups are isomorphic to the wreath products C3wrC2 and C2wrC6 with orders 81 and 384 and with 17 and 28 conjugacy classes respectively, where Cn denotes a cyclic group of order n.展开更多
Self-assembled molecules(SAMs) have shown great potential in replacing bulk charge selective contact layers in high-performance perovskite solar cells(PSCs) due to their low material consumption and simple processing....Self-assembled molecules(SAMs) have shown great potential in replacing bulk charge selective contact layers in high-performance perovskite solar cells(PSCs) due to their low material consumption and simple processing. Herein, we design and synthesize a series of donor-acceptor(D-A) type SAMs(MPA-BTCA, MPA-BT-BA, and MPA-BT-RA, where MPA is 4-methoxy-N-(4-methoxyphenyl)-N-phenylaniline;BT is benzo[c][1,2,5]-thiadiazole;CA is 2-cyanoacrylic acid, BA is benzoic acid, RA is rhodanine-3-propionic acid) with distinct anchoring groups, which show dramatically different properties. MPA-BTCA with CA anchoring groups exhibited stronger dipole moments and formed a homogeneous monolayer on the indium tin oxide(ITO) surface by adopting an upstanding self-assembling mode. However, the MPA-BT-RA molecules tend to aggregate severely in solid state due to the sp~3 hybridization of the carbon atom on the RA group, which is not favorable for achieving a long-range ordered self-assembled layer.Consequently, benefiting from high dipole moment, as well as dense and uniform self-assembled film,the device based on MPA-BT-CA yielded a remarkable power conversion efficiency(PCE) of 21.81%.Encouragingly, an impressive PCE approaching 20% can still be obtained for the MPA-BT-CA-based PSCs as the device area is increased to 0.80 cm^(2). Our work sheds light on the design principles for developing hole selecting SAMs, which will pave a way for realizing highly efficient, flexible, and large-area PSCs.展开更多
Hamiltonian of an O3 molecule is classicized by using coherent states, and its potential energy surface is obtained. The surface and the contours are plotted. The calculated force constants and dissociation energies a...Hamiltonian of an O3 molecule is classicized by using coherent states, and its potential energy surface is obtained. The surface and the contours are plotted. The calculated force constants and dissociation energies are in good agreement with experimental values.展开更多
To rationalize the design of D-π-A type organic small-molecule nonlinear optical materials,a theory guided machine learning framework is constructed.Such an approach is based on the recognition that the optical prope...To rationalize the design of D-π-A type organic small-molecule nonlinear optical materials,a theory guided machine learning framework is constructed.Such an approach is based on the recognition that the optical property of the molecule is predictable upon accumulating the contribution of each component,which is in line with the concept of group contribution method in thermodynamics.To realize this,a Lewis-mode group contribution method(LGC)has been developed in this work,which is combined with the multistage Bayesian neural network and the evolutionary algorithm to constitute an interactive framework(LGC-msBNN-EA).Thus,different optical properties of molecules are afforded accurately and efficientlyby using only a small data set for training.Moreover,by employing the EA model designed specifically for LGC,structural search is well achievable.The origins of the satisfying performance of the framework are discussed in detail.Considering that such a framework combines chemical principles and data-driven tools,most likely,it will be proven to be rational and efficient to complete mission regarding structure design in related fields.展开更多
BrCF_2SO_2Br, prepared from sulfinatodehalogenation of CF_2Br_2 followed by bromination of the intermediate BrCF_2SO_2Na, was shown to be a mild and efficient bromodifluoromethylating agent.
基金supported by the National Natural Science Foundation of China(Nos.22071069,22090050,22176180,21874121 and 21974128)the National Key Research and Development Program of China(Nos.2018YFE0206900 and 2021YFA1200400)+2 种基金Zhejiang Provincial Natural Science Foundation of China under Grant(Nos.LY20B050002 and LD21B050001)Hubei Provincial Natural Science Foundation of China(No.2020CFA037)the Foundation of Basic and Applied Basic Research of Guangdong Province(No.2019B1515120087).
文摘The electrochemical water splitting to produce hydrogen converts electric energy into clean hydrogen energy,which is a groundbreaking concept of energy optimization.To achieve high efficiency,numerous strategies have been developed to enhance the performance of electrocatalysts.Among these,interface engineering with molecules/ions/groups,serves as a versatile approach for optimizing the performance of electrocatalysts in water splitting.On the basis of numerous achievements in high-performance electrocatalysts engineered through molecules/ions/groups at interface,a comprehensive understanding of these advancements is crucial for guiding future progress.Herein,after providing a concise overview of the background,the interface engineering via molecules/ions/groups for electrocatalytic water splitting is demonstrated from three perspectives.Firstly,the engineering of electronic state of electrocatalysts by molecules/ions/groups at interface to reduce the Gibbs free energy of the corresponding reactions.Secondly,the modification of local microenvironment surrounding electrocatalysts via molecules/ions/groups at interface to enhance the transfer of reactants and products.Thirdly,the protection of electrocatalysts with molecule/ion/group fences improves their durability,including protecting active sites from leaching and defending them against harmful species.The fundamental principles of these three aspects are outlined for each,along with pertinent comments.Finally,several research directions and challenges are proposed.
文摘This paper computes the group and character table of Trimethylborane and Cyclohaxane. Results show that the groups are isomorphic to the wreath products C3wrC2 and C2wrC6 with orders 81 and 384 and with 17 and 28 conjugacy classes respectively, where Cn denotes a cyclic group of order n.
基金financial support from the National Natural Science Foundation of China (NSFC)(21805128)the National Natural Science Foundation of China (21774055)+3 种基金the financial support from the National Natural Science Foundation of China(21975260)the Shenzhen Science and Technology Innovation Commission(JCYJ20180504165709042)financial support of Guangdong Provincial Key Laboratory Program(2021B1212040001) from the Department of Science and Technology of Guangdong Provincethe NSFC-CNR exchange program of NSFC(22011530391)。
文摘Self-assembled molecules(SAMs) have shown great potential in replacing bulk charge selective contact layers in high-performance perovskite solar cells(PSCs) due to their low material consumption and simple processing. Herein, we design and synthesize a series of donor-acceptor(D-A) type SAMs(MPA-BTCA, MPA-BT-BA, and MPA-BT-RA, where MPA is 4-methoxy-N-(4-methoxyphenyl)-N-phenylaniline;BT is benzo[c][1,2,5]-thiadiazole;CA is 2-cyanoacrylic acid, BA is benzoic acid, RA is rhodanine-3-propionic acid) with distinct anchoring groups, which show dramatically different properties. MPA-BTCA with CA anchoring groups exhibited stronger dipole moments and formed a homogeneous monolayer on the indium tin oxide(ITO) surface by adopting an upstanding self-assembling mode. However, the MPA-BT-RA molecules tend to aggregate severely in solid state due to the sp~3 hybridization of the carbon atom on the RA group, which is not favorable for achieving a long-range ordered self-assembled layer.Consequently, benefiting from high dipole moment, as well as dense and uniform self-assembled film,the device based on MPA-BT-CA yielded a remarkable power conversion efficiency(PCE) of 21.81%.Encouragingly, an impressive PCE approaching 20% can still be obtained for the MPA-BT-CA-based PSCs as the device area is increased to 0.80 cm^(2). Our work sheds light on the design principles for developing hole selecting SAMs, which will pave a way for realizing highly efficient, flexible, and large-area PSCs.
文摘Hamiltonian of an O3 molecule is classicized by using coherent states, and its potential energy surface is obtained. The surface and the contours are plotted. The calculated force constants and dissociation energies are in good agreement with experimental values.
基金support by the Key Research and Development Program of Zhejiang Province(2023C01102,2023C01208,2022C01208)。
文摘To rationalize the design of D-π-A type organic small-molecule nonlinear optical materials,a theory guided machine learning framework is constructed.Such an approach is based on the recognition that the optical property of the molecule is predictable upon accumulating the contribution of each component,which is in line with the concept of group contribution method in thermodynamics.To realize this,a Lewis-mode group contribution method(LGC)has been developed in this work,which is combined with the multistage Bayesian neural network and the evolutionary algorithm to constitute an interactive framework(LGC-msBNN-EA).Thus,different optical properties of molecules are afforded accurately and efficientlyby using only a small data set for training.Moreover,by employing the EA model designed specifically for LGC,structural search is well achievable.The origins of the satisfying performance of the framework are discussed in detail.Considering that such a framework combines chemical principles and data-driven tools,most likely,it will be proven to be rational and efficient to complete mission regarding structure design in related fields.
文摘BrCF_2SO_2Br, prepared from sulfinatodehalogenation of CF_2Br_2 followed by bromination of the intermediate BrCF_2SO_2Na, was shown to be a mild and efficient bromodifluoromethylating agent.
