可回收反物光一氧化碳化成甲醇＠PEREGRINE科滴

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可回收反物光一氧化碳化成甲醇

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Room-temperature, ambient-pressure conversion reaction for carbon monoxide could be part of a larger cascade strategy for efficiently turning atmospheric carbon dioxide (CO₂) into liquid fuel

一氧化碳於室、境力下的化反可能是，大中二氧化碳(CO₂)，有效化成液燃料之更大策略的一部分。

1. 美布克海文家室及北卡大教堂山分校的研究人了，可再生的有化物，能有效地一氧化碳(CO)化甲醇(CH₃OH)。些反物可能成，大中的二氧化碳(CO₂)化成，易於/存之液燃料的部分策略。

Brookhaven National Laboratory and University of North Carolina Chapel Hill researchers have identified renewable organic hydrides that can efficiently convert carbon monoxide (CO) to methanol (CH₃OH). These reagents could be part of a cascade strategy for converting atmospheric carbon dioxide (CO₂) into easily transportable/storable liquid fuel.

Scientists at the U.S. Department of Energy’s (DOE) Brookhaven National Laboratory and the University of North Carolina Chapel Hill (UNC) have demonstrated the selective conversion of carbon dioxide (CO₂) into methanol using a cascade reaction strategy.

美能源部(DOE)所布克海文家室及北卡大教堂山分校(UNC)的科家已，使用一反策略，性二氧化碳(CO₂)化成甲醇。

The two-part process is powered by sunlight, occurs at room temperature and at ambient pressure, and employs a recyclable organic reagent that’s similar to a catalyst found in natural photosynthesis.

有部分的化程是用一，似在自然光合作用中，被之媒的可回收有反物，在室及境力下，由光所。

“Our approach is an important step toward finding an efficient way to convert CO₂, a potent greenhouse gas that poses a significant challenge for humanity, into an easily storable and transportable liquid fuel,” said Brookhaven Lab Senior Chemist Javier Concepcion, a lead author on the study.

研究主要撰文人，布克海文家室深化家，Javier Concepcion宣：「我的方法是找一，向人成重大挑之有力的室，二氧化碳化成易於存及之液燃料的重要一步。」

The research was conducted as part of the Center for Hybrid Approaches in Solar Energy to Liquid Fuels (CHASE), an Energy Innovation Hub based at UNC and funded by the DOE Office of Science. The study is published as the "front cover" article in the Journal of the American Chemical Society.

表於《美化》，作"封面"文章之研究的行，是部位於北卡大之太能液燃料混合方法中心(CHASE由美能源部科局助之能源新中心)的部分研究。

The room-temperature conversion of CO₂ into liquid fuels has been a decades-long quest. Such strategies could help achieve carbon-neutral energy cycles, particularly if the conversion is powered by sunlight. The carbon emitted as CO₂ by burning single-carbon fuel molecules such as methanol could essentially be recycled into making new fuel without adding any new carbon to the atmosphere.在室下，二氧化碳化成液燃料，已是一十年的探索。此策略可能有助於，碳中和的能源循。特是，倘若是由光所。由於燃如甲醇等，一碳的燃料分子，而以二氧化碳形式排放的碳，本上，能任何新的碳添加到大中，被回收造成新燃料。

Methanol (CH₃OH) is a particularly attractive target because it is a liquid that can be easily transported and stored. In addition to its usefulness as a fuel, methanol serves as a key feedstock in the chemical industry for making more complex molecules.

甲醇(CH₃OH)是一特吸引人的目，因它是一易於及存的液。除了其用作燃料的用外，在造更分子的化工中，甲醇也作一原料。

Also, because methanol contains just one carbon atom, like CO₂, it circumvents the need for making carbon-carbon bonds, which require energy-intensive processes.

However, key steps involved in the reactions required to selectively and efficiently generate solar liquid fuels like methanol remain poorly understood.

此外，由於甲醇二氧化碳一，具有一碳原子。因此，它避了，形成需要能源密集程之碳-碳的需求。然而，在性、有效生，像甲醇等，太能液燃料所需反中，被涉及的步，仍然缺乏被解。

“Converting CO2 to methanol is very difficult to achieve in a single step. It is energetically akin to climbing a very tall mountain,” Concepcion said. “Even if the valley on the other side is at lower altitude, getting there requires a lot of energy input.”

Concepcion宣：「於一步中，很，二氧化碳成甲醇。在能量上，似攀登一座非常高的山。即使，於另一的山谷於低海拔，到那也需要大量的能量入。」

Instead of trying to tackle the challenge in a single “climb,” the Brookhaven/UNC team used a cascade, or multi-step, strategy that goes through several intermediates that are easier to reach. “Imagine climbing several smaller mountains instead of a big one — and doing so through several valleys,” Concepion said.

取代解，於一次“攀登”中的挑。布克海文家室及北卡大的使用了一，容易到之居物的(也就是多重步)策略。Concepion宣：「想像一下，攀登座小而不是一座大山。也就是，穿山谷做到一。」

The valleys represent reaction intermediates. But even reaching those valleys can be difficult, requiring the stepwise exchange of electrons and protons among various molecules. To lower the energy requirements of these exchanges, chemists use molecules called catalysts.

此些山谷代表反居物。不，即使到那些山谷也是困的，需要子及子，在各分子之的逐步交。了降低此些交的能量需求，化家使用被媒的分子。

“Catalysts enable reaching the next valley through ‘tunnels’ that require less energy than climbing over the mountain,” Concepcion said.

Concepcion宣：「媒能透，需要比攀越座山更少能量的‘隧道’，到下一山谷。」

For this study, the team explored reactions employing a class of catalysts called dihydrobenzimidazoles. These are organic hydrides — molecules that have two extra electrons and a proton to “donate” to other molecules. They are inexpensive, their properties can be easily manipulated, and previous studies have shown that they can be recycled, a requirement for a catalytic process.

了研究，研究探索了，使用一被二苯咪唑之媒的反。此些是具有外子及一子，“捐”其他分子的有化物分子。它是廉、性能容易被控制的，且先前多研究已，它能被回收利用，是催化程的一必要件。

These molecules are similar in structure and function to organic cofactors responsible for carrying and delivering energy in the form of electrons and protons during natural photosynthesis.

在及功能上，此些分子在自然光合作用期，以子及子形式，及能量的有因子相似。

“Photosynthesis itself is a cascade of many reaction steps that convert atmospheric CO₂, water, and light energy into chemical energy in the form of carbohydrates — namely sugars — that can later be metabolized to fuel the activity of living organisms. Our approach of using biomimetic organic hydrides to catalyze methanol as a liquid fuel can therefore be viewed as an artificial approach to photosynthesis,” said UNC co-lead author Renato Sampaio.

共同的首要撰文人，北卡大教堂山分校的Renato Sampaio宣：「光合作用本身是一，多反步的，大中的二氧化碳、水及光能化成，之後能被代生物的活，提供燃料之以碳水化合物形式(即醣)的化能。我使用仿生之有化物，催化甲醇作液燃料的方法。因此，能被光合作用的一人工方法。」

In the study, the chemists broke the conversion of CO₂ into methanol into two steps: photochemical reduction of CO₂ to carbon monoxide (CO), followed by sequential hydride transfers from dihydrobenzimidazoles to convert the CO into methanol.

在研究中，此些化家二氧化碳成甲醇的化，分步：CO₂的光化原成一氧化碳(CO)，後二苯咪唑的化物移，CO化成甲醇。

Their work describes the details of the second step, as the reaction proceeds through a series of intermediates, including a ruthenium-bound carbon monoxide (Ru-CO²⁺) group, a ruthenium formyl (Ru-CHO⁺) moiety, a ruthenium hydroxymethyl (Ru-CH₂OH⁺) group, and finally, light-induced methanol release.

他的研究描述了第二步的，反透一系列居物行，包括合了的一氧化碳(Ru-CO₂+)基、甲醯基(Ru-CHO+)部分(成部分中的一部分)、甲基(Ru- CH₂OH+)基及最後，由光的甲醇出。

While the first two steps of this scheme are “dark reactions,” the third step that results in free methanol is initiated by the absorption of light by the ruthenium hydroxymethyl (Ru-CH₂OH⁺) complex.

管此方案的前步是“暗反”，不致游之甲醇的第三步，是由甲基(Ru-CH₂OH+)合物吸收光引的。

The proposed mechanism by which this occurs is through an excited-state electron transfer between the Ru-CH₂OH⁺ and a molecule of organic hydride followed rapidly by a ground proton transfer that results in the generation of methanol in solution.

藉以生被提出的制，是透於Ru-CH₂OH+有化物分子，激的子移，然後快速行致，於溶液中生甲醇的基本子移。

“The ‘one-pot’ and selective nature of this reaction results in the generation of millimolar (mM) concentrations of methanol — the same range of concentrations as the starting materials — and avoids complications that have plagued previous efforts to use inorganic catalysts for these reactions,” said UNC co-author and CHASE Director Gerald Meyer.

合撰人，北卡大教堂山分校兼CHASE(Center for Hybrid Approaches in Solar Energy to Liquid Fuels)主任的Gerald Meyer宣：「反之‘一法’及性的特，致生毫摩(mM)度的甲醇(起始材料相同的度)，且避免了一直使先前多，以使用媒行此些反的。

This work can therefore be viewed as an important step in the use of renewable organic hydride catalysts to the decades-long quest for room temperature catalytic methanol production from CO₂.”