Metal-organic framework-based single-atom electro-/ photocatalysts: Synthesis, energy applications, and opportunities

Single-atom catalysts(SACs)have gained substantial attention because of their exceptional catalytic properties.However,the high surface energy limits their synthesis,thus creating significant challenges for further development.In the last few years,metal–organic frameworks(MOFs)have received significant consideration as ideal candidates for synthesizing SACs due to their tailorable chemistry,tunable morphologies,high porosity,and chemical/thermal stability.From this perspective,this review thoroughly summarizes the previously reported methods and possible future approaches for constructing MOF-based(MOF-derived-supported and MOF-supported)SACs.Then,MOF-based SAC's identification techniques are briefly assessed to understand their coordination environments,local electronic structures,spatial distributions,and catalytic/electrochemical reaction mechanisms.This review systematically highlights several photocatalytic and electrocatalytic applications of MOF-based SACs for energy conversion and storage,including hydrogen evolution reactions,oxygen evolution reactions,O_(2)/CO_(2)/N_(2) reduction reactions,fuel cells,and rechargeable batteries.Some light is also shed on the future development of this highly exciting field by highlighting the advantages and limitations of MOF-based SACs.

电感耦合等离子体原子发射光谱(ICP-AES)法与EDTA滴定法联用测定含白云岩矿石中氟化钙

氟化钙的测定目前较多采用的是国家标准方法GB/T 5195.1—2017和DZG93-05非金属矿萤石分析规程两种方法,前者测定范围≥60%,后者测定范围>3%。两种方法各有优缺点,然而却都无法满足矿石中含有白云岩时的测定。对于萤石矿与白云岩共存样品,直接采用国家标准方法,测定结果偏高,行业标准方法测定的精密度和准确度也很难达到要求。通过对方法进行优化,在样品中加入含钙冰乙酸分离碳酸钙,过滤残渣用混合酸分解后,直接取澄清液在Ca 317.933 nm处,使用电感耦合等离子体原子发射光谱法(ICP-AES)测定氟化钙含量,根据测定结果,将氟化钙质量分数大于15%的样品用EDTA滴定法再次测定。按照实验方法测定实际样品,两种方法测定结果的相对标准偏差(RSD,n=11)分别为1.9%和0.77%,加标回收率为97.9%~102%,可满足含白云岩矿石中氟化钙的准确测定。

Atomic Dispersed Hetero‑Pairs for Enhanced Electrocatalytic CO_(2)Reduction

Electrochemical carbon dioxide reduction reaction(CO_(2)RR)involves a variety of intermediates with highly correlated reaction and ad-desorption energies,hindering optimization of the catalytic activity.For example,increasing the binding of the*COOH to the active site will generally increase the*CO desorption energy.Breaking this relationship may be expected to dramatically improve the intrinsic activity of CO_(2)RR,but remains an unsolved challenge.Herein,we addressed this conundrum by constructing a unique atomic dispersed hetero-pair consisting of Mo-Fe di-atoms anchored on N-doped carbon carrier.This system shows an unprecedented CO_(2)RR intrinsic activity with TOF of 3336 h−1,high selectivity toward CO production,Faradaic efficiency of 95.96%at−0.60 V and excellent stability.Theoretical calculations show that the Mo-Fe diatomic sites increased the*COOH intermediate adsorption energy by bridging adsorption of*COOH intermediates.At the same time,d-d orbital coupling in the Mo-Fe di-atom results in electron delocalization and facilitates desorption of*CO intermediates.Thus,the undesirable correlation between these steps is broken.This work provides a promising approach,specifically the use of di-atoms,for breaking unfavorable relationships based on understanding of the catalytic mechanisms at the atomic scale.

THE ENERGY CRITERION OF MINIMUM EQUIVALENT DIAMETER IN GAS ATOMIZATION

Gas atomization has been studied by using energy method in this paper. It shows that the capillary potential energy of the atomization droplets is supplied by the impingement of the gas on the liquid. The energy criterion of the minimum equivalent diameter of the atomization droplets is obtained. The result is comparable to the empirical formulae.[HJ*2/3]

湿法消解-电感耦合等离子体原子发射光谱(ICP-AES)法测定水凝胶中Mg的含量

为了准确测定水凝胶样品中的金属元素含量,以Mg为例,通过优化电感耦合等离子体原子发射光谱(ICP-AES)仪参数,考察硝酸及硝酸-高氯酸湿法消解以及硝酸-微波消解法对于样品消解程度的不同,建立了湿法消解-ICP-AES法测定水凝胶中Mg绝对含量的方法。结果表明,在110℃下用硝酸消解2 h与硝酸-高氯酸(1∶1)以及硝酸-微波消解得到的溶液相比,Mg含量几乎没有明显差别。在选定条件下,方法的日内和日间精密度良好,相对标准偏差(RSD,n=3)分别为0.38%和1.2%;加标回收率为97.6%~98.2%。方法准确、适用、可靠,适用于水凝胶中Mg的绝对含量测定,可为水凝胶中金属元素的定量分析提供一种借鉴。

Correlation Between Energy Transfer Rate and Atomization Energy of Some Trinitro Aromatic Explosive Molecules

一种假定理论关系被建议在爆炸的开始描述分子的粉碎成原子精力和精力转移率的性质。为了调查在粉碎成原子精力和精力转移之间的关系，评价，炸药的走廊模式的数字被率与正常模式颤动的数字在成正比的 Dlott 和 Fayer 的理论估计。它是借助于密度的八个分子的正常模式颤动的评估频率在 b3p86/6-31G 的功能的理论(DFT )(d， p ) 水平。走廊模式的数字显示出线性关联到分子的粉碎成原子精力，这被发现，它借助于一样的方法也是计算的。这关联的机制被讨论。在有类似的分子的结构和分子的重量的那些炸药，在粉碎成原子精力和走廊模式的数字之间的关联更高，这也被注意。

A novel method for atomization energy prediction based on natural-parameter network

Atomization energy(AE)is an important indicator for measuring material stability and reactivity,which refers to the energy change when a polyatomic molecule decomposes into its constituent atoms.Predicting AE based on the structural information of molecules has been a focus of researchers,but existing methods have limitations such as being time-consuming or requiring complex preprocessing and large amounts of training data.Deep learning(DL),a new branch of machine learning(ML),has shown promise in learning internal rules and hierarchical representations of sample data,making it a potential solution for AE prediction.To address this problem,we propose a natural-parameter network(NPN)approach for AE prediction.This method establishes a clearer statistical interpretation of the relationship between the network’s output and the given data.We use the Coulomb matrix(CM)method to represent each compound as a structural information matrix.Furthermore,we also designed an end-to-end predictive model.Experimental results demonstrate that our method achieves excellent performance on the QM7 and BC2P datasets,and the mean absolute error(MAE)obtained on the QM7 test set ranges from 0.2 kcal/mol to 3 kcal/mol.The optimal result of our method is approximately an order of magnitude higher than the accuracy of 3 kcal/mol in published works.Additionally,our approach significantly accelerates the prediction time.Overall,this study presents a promising approach to accelerate the process of predicting structures using DL,and provides a valuable contribution to the field of chemical energy prediction.

Effects of atomic number Z on the energy distribution of hot electrons generated by femtosecond laser interaction with metallic targets

The effects of atomic number Z on the energy distribution of hot electrons generated by the interaction of 60fs, 130mJ, 800nm, and 7×10^17W/cm^2 laser pulses with metallic targets have been studied experimentally. The results show that the number and the effective temperature of hot electrons increase with the atomic number Z of metallic targets, and the temperature of hot electrons are in the range of 190-230keV, which is consistent with a scaling law of hot electrons temperature.

Chemical Reaction and Energy Transfer Between Hot H Atoms and CO2 Molecules

用时间分辨傅立叶红外发射光谱的方法对H原子与CO2分子的碰撞动力学进行了实验研究．用紫外激光光解的方法分别制备出三个不同平动能为174．7、241．0和306．2 kJ／mol的氢原子,并引发H+CO2→OH+CO反应．观察到了反应的产物,即振动激发的CO (v≤2)．同时也看到了在H原子与CO2分子的碰撞中发生高效的T- V能量转移．CO2的反对称伸缩模的最高振动能级为v=4．化学反应与能量转移的速率之比大约为10．

Wavefunction and energy of the 1s^2 2sns configuration in a beryllium atom

A new set of trial functions for 1s^22sns configurations in a beryllium atom is suggested. A Mathematica program based on the variational method is developed to calculate the wavefunctions and energies of 1s^22sns （n = 3 - 6） configurations in a beryllium atom. Non-relativistic energy, polarization correction and relativistic correction which include mass correction, one- and two-body Darwin corrections, spin-spin contact interaction and orbit-orbit interaction, are calculated respectively. The results are in good agreement with experimental data.

Economic Investigation on the Ultrasonic Atomization Dehumidifying System with Liquid Desiccant and Its Potential Best-Fit Application

The performance of liquid desiccant dehumidification systems can be improved substantially by applying the ultrasonic atomization technology.However,considering the currently-high expense and extra power for the ultrasonic atomizers,it’s unclear if the ultzasonic atomization dehumidifying system(UADS)possesses good economic performance over the conventional packed-bed(PBD)systems.This paper conducted a comparative study on the economic performance between the UADS and PBD.An economic analysis model integrated with the empirical formulae was established while an office building located in Guangzhou,China was employed as the study case.The results indicate the UADS may fit best for buildings with deep-dehumidification needs but smaller-scale areas.

Calculation of Rydberg energy levels for the francium atom

Based on the weakest bound electron potential model theory, the Rydberg energy levels and quantum defects of the nP^2P^o1/2 （n=7-50） and np^2P^o3/2 （n=7-50） spectrum series for the francium atom are calculated. The calculated results are in excellent agreement with the 48 measured levels, and 40 energy levels for highly excited states are predicted.

Solution of the Energy Level of Hydrogen-Like Atom for the Debye Shielding Potential

The first-order revision and the approximation analytical formula of the energy levels for hydrogen-likeatoms under the condition of Debye shielding potential are achieved by means of the Rayleigh-Schrodinger perturbationtheory; meanwhile, the corresponding recurrence relations are obtained from the use of the solution of power series. Basedon the above solutions and with the use of energy consistent method the equivalent value of second-order reversion underthe condition of Debye shielding potential is produced as well and the result is compared with the data obtained by thenumerical method. Besides, the critical bond-state and corresponding cut-off conditions are discussed.

The Quantum Condition That Should Have Been Assumed by Bohr When Deriving the Energy Levels of a Hydrogen Atom

Bohr assumed a quantum condition when deriving the energy levels of a hydrogen atom. This famous quantum condition was not derived logically, but it beautifully explained the energy levels of the hydrogen atom. Therefore, Bohr’s quantum condition was accepted by physicists. However, the energy levels predicted by the eventually completed quantum mechanics do not match perfectly with the predictions of Bohr. For this reason, it cannot be said that Bohr’s quantum condition is a perfectly correct assumption. Since the mass of an electron which moves inside a hydrogen atom varies, Bohr’s quantum condition must be revised. However, the newly derived relativistic quantum condition is too complex to be assumed at the beginning. The velocity of an electron in a hydrogen atom is known as the Bohr velocity. This velocity can be derived from the formula for energy levels derived by Bohr. The velocity v of an electron including the principal quantum number n is given by αc/n. This paper elucidates the fact that this formula is built into Bohr’s quantum condition. It is also concluded in this paper that it is precisely this velocity formula that is the quantum condition that should have been assumed in the first place by Bohr. From Bohr’s quantum condition, it is impossible to derive the relativistic energy levels of a hydrogen atom, but they can be derived from the new quantum condition. This paper proposes raising the status of the previously-known Bohr velocity formula.

Dissipation Energy in Tapping-Mode Atomic Force Microscopes Caused by Liquid Bridge

The dissipation of energy during the process of contact and separation between a tip and a sample is very important for understanding the phase images in the tapping mode of atomic force microscopes（AFMs）. In this study, a method is presented to measure the dissipated energy between a tip and a sample. The experimental results are found to be in good agreement with the theoretical model, which indicates that the method is reliable.Also, this study confirms that liquid bridges are mainly produced by extrusion modes in the tapping mode of AFMs.

Study on the Mathematical Model of Hydraulic Jump Atomization

An equation of atomization quantity from energy dissipation by hydraulic jump was derived from the dimensional analysis. By applying Gauss diffusion equation, the spray diffusion rule in valley was studied under the condition of continuous linear source and random wind direction.By considering the spray rain switching process, coagulation, condensation and evaporation of droplets, the air temperature, air relative humidity, spray density and the rainfall intensity in the lower reaches of the linear source were calculated. The 3 D numerical simulation fitted well with prototype monitoring. Finally, the prediction of atomization influence on environments for Xiangjiaba Hydropower Station was conducted.

Boosting Pseudocapacitive Behavior of Supercapattery Electrodes by Incorporating a Schottky Junction for Ultrahigh Energy Density

Pseudo-capacitive negative electrodes remain a major bottleneck in the development of supercapacitor devices with high energy density because the electric double-layer capacitance of the negative electrodes does not match the pseudocapacitance of the corresponding positive electrodes.In the present study,a strategically improved Ni-Co-Mo sulfide is demonstrated to be a promising candidate for high energy density supercapattery devices due to its sustained pseudocapacitive charge storage mechanism.The pseudocapacitive behavior is enhanced when operating under a high current through the addition of a classical Schottky junction next to the electrode-electrolyte interface using atomic layer deposition.The Schottky junction accelerates and decelerates the diffusion of OH-/K+ions during the charging and discharging processes,respectively,to improve the pseudocapacitive behavior.The resulting pseudocapacitive negative electrodes exhibits a specific capacity of 2,114 C g^(-1)at 2 A g^(-1)matches almost that of the positive electrode’s 2,795 C g^(-1)at 3 A g^(-1).As a result,with the equivalent contribution from the positive and negative electrodes,an energy density of 236.1 Wh kg^(-1)is achieved at a power density of 921.9 W kg^(-1)with a total active mass of 15 mg cm-2.This strategy demonstrates the possibility of producing supercapacitors that adapt well to the supercapattery zone of a Ragone plot and that are equal to batteries in terms of energy density,thus,offering a route for further advances in electrochemical energy storage and conversion processes.

DETERMINATION OF THE SURFACE BINDING ENERGY OF A Cu/Li ALLOY BY MEASUREMENTS OF ANGULAR DISTRIBUTION OF SPUTTERED ATOMS

A copper based binary alloy containing 16.9 at % lithium has been bombarded with deuterium ions in energy range of 400 eV to 2 keV at the incidence angles of 70° and 80° away from the surface normal. The sputtered flux was condensed on Al- strips arranged arround the target in a cylindrical cup. 1.5 MeV proton backscattering and nuclear reaction 7Li(p, α)4He were used to detect the collected atoms of Cu and Li simultaneously. The angular distribution of sputtered atoms has been shown to be different for two components and strongly anisotropic for the grazing incidence. According to direct knock-on sputtering model and the experimental results the angle for the maximum differential sputtering yield is dependent on the incidence angle α, the bombarding energy E, the energy transfer factor γ= 4M1M2/(M1+ M2)2 and the surface binding energy U. With the assumption that the sputtered particles are diffracted by a planar barrier the surface binding energies of 2.3 eV for the Li component and 3.0 eV for the Cu component have been determined by fitting the measured angles of preferred ejection to the direct knock-on sputtering model, and the results agree well with a pair-binding model.

Stable High-Energy Density Super-Atom Clusters of Aluminum Hydride

与这个概念超级原子，第一原则计算建议比很好确定的簇是更多精力充沛的马厩的超级稳定的笼子簇 AlnH3n 的一种新类型， AlnHn+2。在新簇，铝核心框架是行动一与 n 顶点和 2n Al-Al 边超级原子，它允许吸附 n 氢原子在最高地点并且在桥地点的 2n。把 Al12H36 用作基本单位，稳定的链结构，(Al12H36 ) m，被构造了跟随一样的连接机制至于(AlH3 ) n 线性聚合结构。除了高氢百分比每分子，计算证明了这些新簇拥有形成价值的大热，他们的燃烧热是大约 4.8 次甲烷，使他们成为有希望的高精力密度材料。

Molecular Dynamics Study on Interfacial Energy and Atomic Structure of Ag/Ni and Cu/Ni Heterophase System

The results of molecular dynamics calculations on the interfacial energies and atomic structures of Ag/Ni and Cu/Ni interfaces are presented. Calculation on Ag/Ni interfaces with low-index planes shows that those containing the (111) plane have the lowest energies, which is in agreement with the experiments. Comparing surface energy with interfacial energy, it is found the order of the interfacial energies of Ag/Ni and Cu/Ni containing the planes fall in the same order as solid-vapor surface energies of Ag, Cu and Ni. In this MD simulation, the relaxed atomic structure and dislocation network of (110)_Ag||(110)Ni interface are coincident to HREM observations.