Molecular Engineering of Cation Solvation Structure for Highly Selective Carbon Dioxide Electroreduction

Balancing the activation of H₂O is crucial for highly selective CO₂ electroreduction (CO₂RR), as the protonation steps of CO₂RR require fast H₂O dissociation kinetics, while suppressing hydrogen evolution (HER) demands slow H₂O reduction. We herein proposed one molecular engineering strategy to regulate the H₂O activation using aprotic organic small molecules with high Gutmann donor number as a solvation shell regulator. These organic molecules occupy the first solvation shell of K⁺ and accumulate in the electrical double layer, decreasing the H₂O density at the interface and the relative content of proton suppliers (free and coordinated H₂O), suppressing the HER. The adsorbed H₂O was stabilized via the second sphere effect and its dissociation was promoted by weakening the O−H bond, which accelerates the subsequent *CO₂ protonation kinetics and reduces the energy barrier. In the model electrolyte containing 5 M dimethyl sulfoxide (DMSO) as an additive (KCl-DMSO-5), the highest CO selectivity over Ag foil increased to 99.2 %, with FE_CO higher than 90.0 % within −0.75 to −1.15 V (vs. RHE). This molecular engineering strategy for cation solvation shell can be extended to other metal electrodes, such as Zn and Sn, and organic molecules like N,N-dimethylformamide.     

磷钼钨杂多酸修饰金属有机骨架MOF-5复合材料吸附亚甲基蓝

采用水热合成法,在合成金属有机骨架MOF-5的过程中引入活性组分磷钼钨杂多酸(H₆P₂Mo₁₅W₃O₆₂),制备出一种新型吸附剂H₆P₂Mo₁₅W₃O₆₂/MOF-5。 利用H₆P₂Mo₁₅W₃O₆₂/MOF-5材料对亚甲基蓝溶液进行了材料的吸附性能研究,探讨了亚甲基蓝溶液的初始pH值和初始浓度以及不同吸附温度对吸附量的影响。 结果表明,在较低的温度和亚甲基蓝溶液较低的初始pH值的条件下,有利于H₆P₂Mo₁₅W₃O₆₂/MOF-5对亚甲基蓝的吸附。 实验结果能够较好地符合Langmuir吸附等温式以及二级动力学模型,对亚甲基蓝的最大吸附量可达401.6 mg/g。 热力学参数ΔG<0、ΔH<0和ΔS>0,表明H₆P₂Mo₁₅W₃O₆₂/MOF-5对亚甲基蓝的吸附过程是自发、放热的。 此外,还探讨了H₆P₂Mo₁₅W₃O₆₂/MOF-5对甲基紫、孔雀石绿、罗丹明B和甲基橙等其它染料的吸附性能,结果表明,H₆P₂Mo₁₅W₃O₆₂/MOF-5对阳离子染料有较好的吸附效果。     

On the general Kloosterman sum and its fourth power mean

The main purpose of this paper is to study the asymptotic property of the fourth power mean of the general Kloosterman sums, and give an interesting calculating formula.     

关于设计距离为7的BCH码的非循环等价类

利用Mobius公式给出了设计距离为7的二元BCH码的非循环等价类的精确计数．     

关于Dedekind和的均值公式

本文的主要目的是利用ＤｉｒｉｃｈｌｅｔＬ－函数的均值定理研究Ｄｅｄｅｋｉｎｄ和的值分布性质，并给出一个较强的均值公式．     

On Lehmer’s problem and Dedekind sums

Let p be an odd prime and c a fixed integer with (c, p) = 1. For each integer a with 1 ≤ a ≤ p ? 1, it is clear that there exists one and only one b with 0 ? b ? p ? 1 such that ab ≡ c (mod p). Let N(c, p) denote the number of all solutions of the congruence equation ab ≡ c (mod p) for 1 ? a, b ? p?1 in which a and \(\overline b \) are of opposite parity, where \(\overline b \) is defined by the congruence equation b\(\overline b \) ≡ 1 (mod p). The main purpose of this paper is to use the properties of Dedekind sums and the mean value theorem for Dirichlet L-functions to study the hybrid mean value problem involving N(c, p)?½φ(p) and the Dedekind sums S(c, p), and to establish a sharp asymptotic formula for it.