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首页> 外文期刊>Biophysical Chemistry: An International Journal Devoted to the Physical Chemistry of Biological Phenomena >The maximum entropy production requirement for proton transfers enhances catalytic efficiency for beta-lactamases
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The maximum entropy production requirement for proton transfers enhances catalytic efficiency for beta-lactamases

机译：质子转移的最大熵产量要求增强了β-内酰胺酶的催化效率

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摘要

Movement of charges during enzyme catalytic cycle may be due to conformational changes, or to fast electron or proton transfer, or to both events. In each case, entropy production can be calculated using Terrel L. Hill's method, if relevant microscopic rate constants are known. When ranked by their evolutionary distance from putative common ancestor, three beta-lactamases considered in this study show correspondingly increased catalytic constant, catalytic efficiency, and overall entropy production. The acylation and deacylation steps with concomitant proton shuttles are the most important contributors to overall entropy production. The maximal entropy production requirement for the ES - EP or Ep - E + P step leads to optimal rate constants, performance parameters, and entropy production values, which are close to those extracted from experiments and also rank in accordance with evolutionary distances. Concurrent maximization of entropy productions for both proton transfer steps revealed that evolvability potential of different beta-lactamases is similarly high. These results may have implications in particular for latent potential of beta-lactamases to evolve further and in general for selection of optimized enzymes through natural or directed evolution.
机译：酶催化循环期间电荷的运动可能是由于构象变化，或快速电子或质子转移，或两种事件。在每种情况下，如果已知相关的微观速率常数，则可以使用Terrel L. Hill的方法计算熵产生。当通过从推定的共同祖先的进化距离排名时，本研究中考虑的三种β-内酰胺酶显示出相应地增加了催化恒定，催化效率和整体熵产生。具有伴随质子班车的酰化和脱酰化步骤是对整体熵产生的最重要的贡献者。 ES＆ - ＆gt的最大熵生产要求。 EP或EP＆ - ＆ E + P步骤导致最佳的速率常数，性能参数和熵产生值，靠近实验中提取的那些，并且还按照进化距离排列。两种质子转移步骤的熵制剂的同时最大化显示出不同β-内酰胺酶的再溶解性电位类似地高。这些结果可能对β-内酰胺酶的潜在潜在来说有影响，以进一步发展，并且通常通过天然或定向的进化选择优化的酶。

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