摘要：铂(Pt)是质子交换膜燃料电池(PEMFCs)阳极氢氧化反应(HOR)中最先进的电催化剂.然而,Pt催化剂对CO(工业低成本氢燃料中的杂质)极度敏感从而中毒,这会引起器件性能的急剧衰退,导致器件运行成本高.因此,提高Pt催化剂的CO耐受性对PEMFCs的商业化推广至关重要.在此,我们设计合成了一种独特的PtNiW@WO_(x)核壳纳米线来提高Pt基催化剂对CO的耐受能力.机理研究表明,表面无定形的WO_(x)壳层可以作为分子围栏,在动力学上阻碍CO扩散到达Pt位点.在热力学上,Ni和W元素合金化产生的电子效应可以使Pt的d带中心降低,减弱CO在Pt位点上的化学吸附.此外,亲氧W元素可以加速水的解离,提供更多OH活性物种,促进CO的氧化脱附.因此,在1000ppm CO/H_(2)条件下,所设计的PtNiW@WO_(x)核壳纳米线催化剂表现出优异的HOR抗CO中毒性能,在4000 s后仍能保持超过90%的HOR电流密度,超过了原始的PtNi纳米线和目前报道的绝大多数Pt基催化剂.

摘要：净零能耗(NZE)建筑的能源来源于清洁的可再生资源。本文以一个包含一个足球场和两个游泳池的体育中心为研究对象,基于净零能耗(NZE)概念对体育中心进行设计和分析。虽然这类体育中心很常见,但针对这类体育中心开发净零能耗系统的研究却非常有限。在体育中心的屋顶上安装了10000 m^(2)的太阳能光伏板,提供其所需的能量。白天产生的能量通过压缩空气储能(CAES)循环储存起来,在日落后按需使用。压缩空气驱动涡轮机,为体育中心提供所需的电力;同时,产生的热能被用来加热游泳池;利用环境和气象数据进行瞬态研究。利用TRNSYS软件进行了动态模拟;结果表明,该循环的总效率约为44%,如果使用游泳池的热能,则可提高到98%。由于太阳能的波动,平均所需能源的14%应由电网提供,且每天可出售超过26 MW·h的能源到电网。这项研究的结果有助于设计NZE运动场馆,实现能源的可持续管理。

摘要：LASP(large-scale atomistic simulation with neural network potential)software developed by our group since 2018 is a powerful platform(***)for performing atomic simulation of complex *** software integrates the neural network(NN)potential technique with the global potential energy surface exploration method,and thus can be utilized widely for structure prediction and reaction mechanism *** we introduce our recent update on the LASP program version 3.0,focusing on the new functionalities including the advanced neuralnetwork training based on the multi-network framework,the newly-introduced S^(7) and S^(8) power type structure descriptor(PTSD).These new functionalities are designed to further improve the accuracy of potentials and accelerate the neural network training for multipleelement *** Cu-C-H-O neural network potential and a heterogeneous catalytic model as the example,we show that these new functionalities can accelerate the training of multi-element neural network potential by using the existing single-network potential as the *** obtained double-network potential Cu CHO is robust in simulation and the introduction of S^(7) and S^(8) PTSDs can reduce the root-mean-square errors of energy by a factor of two.

摘要：The nitrogen reduction reaction(NRR)using new and efficient electrocatalysts is a promising al‐ternative to the traditional Haber‐Bosch ***,it remains a challenge to design efficient catalysts with improved catalytic ***,various O‐functional MXenes were investigated as NRR catalysts by a combination of density functional theory calculations and least absolute shrinkage and selection operator(LASSO)***_(3)C_(2)O_(X) has been regarded as a promising catalyst for the NRR because of its stability,activity,and *** poten‐tial‐determining step is*NH_(2) hydrogenation to*NH3 with a limiting potential of-0.45 ***‐more,via LASSO regression,the descriptors and equations fitting the relationship between the properties of O‐functional MXenes and NRR activity have been *** work not only pro‐vides a rational design strategy for catalysts but also provides machine learning data for further investigation.

摘要：This vertically self‐pillared(VSP)structure extends the application range of traditional porous materials with facile mass/ion transport and enhanced reaction ***,we prepare a single crystal metal‐organic framework(MOF),employing the ZIF‐67 structure as a proof of concept,which is constructed by vertically self‐pillared nanosheets(VSP‐MOF).We further converted VSP‐MOF into VSP‐cobalt sulfide(VSP‐CoS2)through a sulfidation *** plays an important role in almost all battery technologies;for metallic batteries,lithium anodes exhibit a high theoretical specific capacity,low density,and low redox ***,during the half‐cell reaction(Li++e=Li),uncontrolled dendritic Li penetrates the separator and solid electrolyte interphase *** employed as a composite scaffold for lithium metal deposition,there are many advantage to using this framework:1)the VSP‐CoS2 substrate provides a high specific surface area to dissipate the ion flux and mass transfer and acts as a pre‐catalyst,2)the catalytic Co center favors the charge transfer process and preferentially binds the Li+with the enhanced electrical fields,and 3)the VSP structure guides the metallic propagation along the nanosheet 2D orientation without the protrusive *** these features enable the VSP structure in metallic batteries with encouraging performances.

摘要：Herein,we report a three-dimensional porous TiO_(2)/Fe_(2)TiO_(5)/Fe_(2)O_(3)(TFF)inverse opal through in situ thermal solid reactions for photoelectrochemical water *** Fe_(2)TiO_(5) interfacial layer within TFF acting as a bridge to tightly connect to TiO_(2) and Fe_(2)O_(3) reduces the interfacial charge transfer resistance,and suppresses the bulk carrier *** optimized TFF displays a remarkable photocurrent density of 0.54mAcm^(-2) at 1.23V *** hydrogen electrode(RHE),which is 25 times higher than that of TiO_(2)/Fe_(2)O_(3)(TF)inverse opal(0.02mAcm^(-2) at 1.23V ***).The charge transfer rate in TFF inverse opal is 2-8 times higher than that of TF in the potential range of 0.7-1.5V *** effects of the Fe_(2)TiO_(5) interfacial layer are further revealed by X-ray absorption spectroscopy and intensity-modulated photocurrent *** work offers an interfacial engineering protocol to improve charge separation and transfer for efficient solar water splitting.

摘要：Negative thermal expansion(NTE),as an abnormal physical behavior,has been followed by scientists’attention over the past 30 years,due to its fascinating physical mechanisms and the prospect of high-precision thermal expansion control[1-5].Although some NTE materials(alloys[6],cyanides[7],fluorides[8-10],nitrides[11],oxides[12,13],MOFs[14-16],etc.)have been found,their number and variety are still very small,limiting their *** and designing new NTE materials is an important and challenging topic for the development of the field of *** have been continually reviewing and summarizing obtained results to look to the future of NTE[17-23].

摘要：Each conventional alloy has its own specific compositions but the compositional origin is largely unknown due to our insufficient understanding about chemical shortrange ordering in the alloy,in particular,in the solid-solution *** the present paper,the compositions of metallic alloys are discussed and formulated,by unveiling the basic moleculelike structural units in solid *** oscillation theory,which describes the partial charge screening behavior in solid solutions,and henceforth the origin of short-range ordering,is applied to pin down the ideal chemical compositions of conventional metallic *** propose that,at a specific composition,atoms self-assemble into an ideally ordered structure consisting of atoms residing in the nearestneighbor shell(denoted as cluster)plus those in the next outer shell(denoted as glue atoms),which can be formulated as[cluster](glue atoms).This simplified version of short-rangeorder structure represents the smallest charge-neutral and mean-density zone(termed as“chemical units”)and can be regarded as the‘molecules’of solid ***,the chemical units and the corresponding molecule-like formulas for face-centered-cubic(FCC),hexagonal close-packed(HCP),and body-centered cubic(BCC)structures are analyzed and equations are obtained to identify the chemical formulas for FCC solid *** instance,well-knownα-brass Cu-30 Zn alloy is formulated as[Zn-Cu_(12)]*** of aluminum alloys,superalloys and stainless steels are also illustrated,demonstrating the versatility of the present model to interpret chemically complex alloys.

摘要：量子自旋霍尔绝缘体拥有具有带隙的体态和无能隙的一维拓扑边缘态.然而,由于拓扑边缘态局域在纳米尺度,所以很难用光学手段直接观测并区分体态和边缘态,这就限制了对拓扑边缘态独特的光学特性和光电响应等方面的研究和应用.Bi_(4)Br_(4)体材料的台阶存在一维非平庸的边缘态,多个台阶累加的效应使得通过较为宏观的光学和光电分析手段来研究一维边缘态成为可能.该工作利用中远红外显微吸收光谱和泵浦探测光谱,对比研究了Bi_(4)Br_(4)体和边缘的光学响应行为.研究发现Bi_(4)Br_(4)的边缘在小于带隙(约0.22 eV)的波段存在明显的强于体内的红外吸收,且该吸收呈现较强的各向异性.室温下的红外泵浦探测首次观察到边缘处载流子激发态超长的弛豫时间(1.5 ns),该激发态载流子寿命要比体内载流子寿命长两个量级.该工作证实体态和拓扑边缘态具有明显不同的光学和光电响应行为,为未来设计新型红外探测器提供了材料和物理基础.